Multiscale Assembly Research Articles

Engineered Protein Fibers with Reinforced Mechanical Properties Via β-Sheet High-Order Assembly.

Protein fibers are ideal alternatives to synthetic polymers due to their unique mechanical properties, biocompatibility, and sustainability. However, engineering biomimetic protein fibers with high mechanical properties remains challenging, particularly in mimicking the high molecular weight of natural proteins and regulating their complex hierarchical structures. Here, a modular design and multi-scale assembly strategy is developed to manufacture robust protein fibers using low- or medium-molecular-weight proteins. The distinct functional and structural properties of flexible, rigid, and cross-linked domains in modular proteins are skillfully harnessed. By regulating the ratio of rigid to flexible domains, the formation of high-order β-sheet crystals aligned along the fiber axis is promoted, enhancing both strength and toughness. Furthermore, the dynamic imine cross-linking network, formed by the aldehyde-amine condensation reaction of the cross-linked domains, further reinforces the protein fibers. Remarkably, fibers spun from modular proteins significantly smaller than natural spidroin exhibit outstanding mechanical properties, surpassing those of protein fibers with same or even higher molecular weights. This strategy offers a promising pathway for fabricating protein fibers suitable for diverse applications.

Bringing multiscale dot-sheet heterostructured assembly into lignin valorization for efficient water desalination and zinc-ion hybrid capacitors

The notion of biomass valorization has been widely adopted to alleviate low-carbon-emission anxieties with the attributes in energy-environmental sustainability via groping multiscale-structured composite, yet still suffering from the dilemma of lignin upcycling. In this context, we propose a novel dot-sheet-assembled heterostructure featuring all lignin-derived bifunctional carbon composites (Co-N-C@CDs) that includes porous Co, N co-modified nanosheets and solvent-extracted carbon quantum dots. The photo-physical properties of lignin-based CDs are refined into multicolor green- and red-emissive fractions (GCDs and RCDs) via a facile biphasic fractionation. Owing to the high-graphite and conductivity, the red-emitting RCDs are installed with lamellar Co-N-C to favor the enlarged interlayer spacing, fast ionic intercalation-transfer and reversible chemical adsorption, thereby resulting in high-performance capacitive deionization (CDI) and zinc-ion hybrid capacitors (ZIHCs). While assembling the CDI device, the Co-N-C@CDs possess a maximum adsorption capacity of 33.64 mg g−1 NaCl in water desalination with stable restorable behavior. As the cathode of ZIHCs, it delivers an operating voltage of 2.0 V and superior energy density of 209.72 Wh kg−1, posing a long-term cycling durability at high current rates. Detailed hierarchical structure readily enables the large specific surface area, excellent percolating porosity, intercalated hydrogen bonds and redox active sites, which are conducive to not only expedite ionic infiltration and charge reaction kinetics but also reduce the energy barriers of aqueous ion adsorption. The multiscale 0D-2D supramolecular assembly breaks the frontier of lignin valorization to connecting energy-environment functions, thereby meeting the needs of carbon–neutral society.

Chitin/Chitosan Nanofibers Toward a Sustainable Future: From Hierarchical Structural Regulation to Functionalization Applications.

Owing to its multiple fascinating properties of renewability, biodegradability, biocompatibility, and antibacterial activity, chitin is expected to become a green cornerstone of next-generation functional materials. Chitin nanofibers, as building blocks, form multiscale hierarchical structures spanning nano- and macrolevels in living organisms, which pave the way for sophisticated functions. Therefore, from a biomimetic perspective, exploiting chitin nanofibers for use in multifunctional, high-performance materials is a promising approach. Here, we first summarize the latest advances in the multiscale hierarchical structure assembly mode of chitin and its derivative nanofibers, including top-down exfoliation and bottom-up synthesis. Subsequently, we emphasize the environmental impacts of these methods, which are crucial for whether chitin nanofibers can truly contribute to a more eco-friendly era. Furthermore, the latest progress of chitin nanofibers in environmental and medical applications is also discussed. Finally, the potential challenges and tailored solutions of chitin nanofibers are further proposed, covering raw material, structure, function, manufacturing, policies, etc.

Symmetry-Guided Inverse Design of Self-Assembling Multiscale DNA Origami Tilings.

Recent advances enable the creation of nanoscale building blocks with complex geometries and interaction specificities for self-assembly. This nearly boundless design space necessitates design principles for defining the mutual interactions between multiple particle species to target a user-specified complex structure or pattern. In this article, we develop a symmetry-based method to generate the interaction matrices that specify the assembly of two-dimensional tilings, which we illustrate using equilateral triangles. By exploiting the allowed 2D symmetries, we develop an algorithmic approach by which any periodic 2D tiling can be generated from an arbitrarily large number of subunit species, notably addressing an unmet challenge of engineering 2D crystals with periodicities that can be arbitrarily larger than the subunit size. To demonstrate the utility of our design approach, we encode specific interactions between triangular subunits synthesized by DNA origami and show that we can guide their self-assembly into tilings with a wide variety of symmetries, using up to 12 unique species of triangles. By conjugating specific triangles with gold nanoparticles, we fabricate gold-nanoparticle supracrystals whose lattice parameter spans up to 300 nm. Finally, to generate economical design rules, we compare the design economy of various tilings. In particular, we show that (1) higher symmetries allow assembly of larger unit cells with fewer subunits and (2) linear supracrystals can be designed more economically using linear primitive unit cells. This work provides a simple algorithmic approach to designing periodic assemblies, aiding in the multiscale assembly of supracrystals of nanostructured "meta-atoms" with engineered plasmonic functions.

Spontaneous Multi-scale Supramolecular Assembly Driven by Noncovalent Interactions Coupled with the Continuous Marangoni Effect.

Reported herein is the multi-scale supramolecular assembly (MSSA) process along with redox reactions driven by supramolecular interactions coupled with the spontaneous Marangoni effect in ionic liquid (IL)-based extraction systems. The black powder, the single sphere with a black exterior, and the single colorless sphere were formed step by step at the interface when an aqueous solution of KMnO4 was mixed with the IL phase 1-(2-hydroxyethyl)-3-methylimidazolium bis(trifluoromethylsulfonyl) imide (C2OHmimNTf2) bearing octyl(phenyl)-N,N-diisobutylcarbamoylmethylphosphine oxide (CMPO). The mechanism of the whole process was studied systematically. The phenomena were related closely to the change in the valence state of Mn. The MnO4- ion could be reduced quickly to δ-MnO2 and further to Mn2+ slowly by the hydroxyl-functionalized IL C2OHmimNTf2. Based on Mn2+, Mn(CMPO)32+, elementary building blocks (EBBs), and [EBB]n clusters were generated step by step. The [EBB]n clusters with the large enough size that were transferred to the interface, together with the remaining δ-MnO2, assembled into the single sphere with a black exterior, driven by supramolecular interactions coupled with the spontaneous Marangoni effect. When the remaining δ-MnO2 was used up, the mixed single sphere turned completely colorless. It was found that the reaction site of C2OHmim+ with Mn(VII) and Mn(IV) was distributed mainly at the side chain with a hydroxyl group. The MSSA process presents unique spontaneous phase changes. This work paves the way for the practical application of the MSSA-based separation method developed recently. The process also provides a convenient way to observe in situ and characterize directly the continuous Marangoni effect.

Hierarchically Superstructured Anisotropic Carbon Particles by Multiscale Assembly Driven by Spinodal Decomposition.

Hierarchical superstructures have novel shape-dependent properties, but well-defined anisotropic carbon superstructures with controllable size, shape, and building block dimensionality have rarely been accomplished thus far. Here, a hierarchical assembly technique is presented that uses spinodal decomposition (SD) to synthesize anisotropic oblate particles of mesoporous carbon superstructure (o-MCS) with nanorod arrays by integrating block-copolymer (BCP) self-assembly and polymer-polymer interface behaviors in binary blends. The interaction of major and minor phases in binary polymer blends leads to the formation of an anisotropic oblate particle, and the BCP-rich phase enables ordered packing and unidirectional alignment of carbon nanorods. Consequently, this approach enables precise control over particles' size, shape, and over the dimensionality of their components. Exploiting this functional superstructure, o-MCS are used as an anode material in potassium-ion batteries, and achieve a notable specific capacity of 156mAhg-1 at a current density of 2Ag-1, and long-term stability for 3000 cycles. This work presents a significant advancement in the field of hierarchical superstructures, providing a promising strategy for the design and synthesis of anisotropic carbon materials with controlled properties, offering promising applications in energy storage and beyond.

Autofluorescence microscopy as a non-invasive probe to characterize the complex mechanical properties of keratin-based integumentary organs: A feather paradigm

Integumentary organs exhibit diverse morphologies and functions. The complex mechanical property of the architecture is mainly contributed by the ingenious multiscale assembly of keratins. A cross-scale characterization on keratin integration in an integument system will help us understand the principles on how keratin-based bio-architecture are built and function in nature. In this study, we used feather as a model integument organ. We develop autofluorescence (AF) microscopy to study the characteristics of its keratin assemblies over a wide range of length scales. The AF intensity of each feather component, following the hierarchy from the rachis to barb to barbule, decreased with the physical dimension. By combining the analysis of AF signal and tensile testing, we can probe regional material density and the associated mechanical strength in a composite feather. We further demonstrated that the AF micro-images could resolve subtle variations in the defective keratin assembly in feathers from frizzled chicken variants with a mutation in α-keratin 75. The distinction between AF patterns and the morphological features of feather components across different length scales indicated a synergetic interplay between material integration and complex morphogenesis during feather development. The work shows AF microscopy can serve as an easy and non-invasive approach to study multiscale keratin organizations and the associated bio-mechanical properties in diverse integumentary organs. This approach will facilitate our learning of many bio-inspired designs in diverse animal integumentary organs/appendages.

Multi-Scale Altitudinal Patterns of Soil and Litter Invertebrate Communities in a Warm Temperate Deciduous Broadleaf Forest

The diversity and spatial patterns of soil invertebrates are the cornerstones for understanding their ecological functions, which are crucial to maintaining nutrient cycling and soil health in forest ecosystems. Based on a continuous altitudinal gradient (1020–1770 m) composed of 119 plots, this study analyzed the spatial patterns of invertebrate communities in temperate mountain forest litter and soil using multi-scale ordination. The results indicate that along the altitudinal gradient, the invertebrate communities in both litter and soil layers exhibit “patches” at a scale of approximately 33 plots that are mainly composed of Mesostigmata and Apterogasterine oribatid mites. In the litter layer, at the 11-plot scale, an aggregation of Onychiuridae is also formed, while in the soil layer, there are “patches” represented by Diadocidiidae at the 33-plot scale. The positive–negative associations among invertebrate taxa also shift between the litter and soil layers, as well as among “patches”. Our study confirms that the richness of invertebrates in temperate-forest litter is higher and forms multi-scale assembly “patches” despite the higher abundance of invertebrates in the soil layer. Future studies should delve deeper into the aggregation mechanisms of these specific taxa and may require higher sampling densities to reveal the multi-scale spatial patterns of soil invertebrates.

Three‐dimensional multiscale assembly of phyllosilicates, organics, and carbonates in small Ryugu fragments

AbstractWe report μm‐scale nondestructive infrared (IR) hyperspectral results (IR computed tomography, IR‐CT) in 3‐D and IR surface imaging, IR‐S) in 2‐D, at SOLEIL) combined with X‐ray nano‐computed tomography analyses (at SPring‐8) performed on eight small Ryugu fragments extracted from mm‐sized grains coming both from touchdown first and second sites. We describe the multiscale assembly of phyllosilicates, carbonates, sulfides, oxides, and organics. Two types of silicates, as well as diverse kinds of organic matter, were detected inside Ryugu material. Their spatial correlations are described to discuss the role of the mineralogical microenvironments in the formation/evolution of organic matter. In particular, we have shown that there is a redistribution of the organic matter diffuse component during aqueous alteration on the parent body, with a preferential circulation among fine‐grained phyllosilicates.

Assembly and Characterization of Length-Sorted, Aligned Boron Nitride/Carbon Nanotube Thin Film Composites Via Slow Vacuum Filtration

Globally aligned single-wall carbon nanotubes (SWCNTs) are a promising, scalable platform for studying fundamental physical phenomena and an important vehicle for optoelectronic device applications. Recent work by Rust et al. [1] has identified nanotube length as an important mediating factor in the degree and scale of SWCNT alignment via slow vacuum filtration (SVF).Building on this work and that of Walker et al. [2,3], we explore the co-assembly of length-sorted SWCNTs and boron nitride nanotubes (BNNTs) atop polycarbonate track-etched membranes. BNNTs have recently gained interest as a chirality-agnostic, wide-bandgap material for encapsulation, insulation, thermal/mechanical robustness, and visible-light transparency, while also having a similar high aspect ratio morphology, making them an exceptional and alignable host matrix for individualized CNT species. To prepare such hybrid assemblies, a polymer-assisted, depletion-based method was first used to length-sort different diameter SWCNT (alkane filled electric-arc, CoMoCAT, metallic-sorted Tuball), and BNNT nanotube populations. Thereafter, we investigated the impacts of tube lengths, relative BN/C fraction, mass loading, and presence of a global director force on the multi-scale assembly behavior. A combination of birefringence microscopy and polarized Raman spectroscopy probed and identified trends in global and local ordering under these conditions.[1] Rust, C., Shapturenka, P., Spari, M., Jin, Q., Li, H., Bacher, A., Guttmann, M., Zheng, M., Adel, T., Hight Walker, A. R., Fagan, J. A., & Flavel, B. S. (2022). The Impact of Carbon Nanotube Length and Diameter on their Global Alignment by Dead-End Filtration. Small (forthcoming).[2] Walker, J. S., Fagan, J. A., Biacchi, A. J., Kuehl, V. A., Searles, T. A., Hight Walker, A. R., & Rice, W. D. (2019). Global Alignment of Solution-Based Single-Wall Carbon Nanotube Films via Machine-Vision Controlled Filtration. Nano Letters, 19(10), 7256–7264.[3] Walker, J. S., Macdermid, Z. J., Fagan, J. A., Kolmakov, A., Biacchi, A. J., Searles, T. A., Walker, A. R. H., & Rice, W. D. (2022). Dependence of Single‐Wall Carbon Nanotube Alignment on the Filter Membrane Interface in Slow Vacuum Filtration. Small, 18, 2105619.

Improvement on the Radiation Stability of Multi-scale Supramolecular Assembly in Ionic Liquid-Based Extraction.

The multi-scale supramolecular assembly (MSSA)-based extraction strategy with hydroxyl-functionalized ionic liquid (IL) is promising in the separation of metal ions from radioactive environments for which a comprehensive understanding toward the radiation stability of the MSSA system is necessary. Herein, we report on the analyses of the radiation stability of MSSA in extraction, especially the adopted ILs 1-(2-hydroxyethyl)-3-methylimidazolium bis(trifluoromethylsulfonyl) imide (IL-1) and 1-(2-hydroxyethyl)-2,3-dimethylimidazolium bis(trifluoromethylsulfonyl) imide (IL-2), by UV-vis, 1H NMR, and ESI-HRMS. It was found that the macroscopic assembly (MA) sphere could not be formed after γ irradiation on the extraction system with IL-1. On the contrary, the trisubstituted IL-2 instead of the disubstituted IL-1 remarkably improved the radiation stability of the MSSA system to guarantee the formation of the MA sphere. The high extraction efficiency could be kept, and the mechanism of such an improvement was revealed.

Recent Experimental Advances in Characterizing the Self-Assembly and Phase Behavior of Polypeptoids.

Polypeptoids are a family of synthetic peptidomimetic polymers featuring N-substituted polyglycine backbones with large chemical and structural diversity. Their synthetic accessibility, tunable property/functionality, and biological relevance make polypeptoids a promising platform for molecular biomimicry and various biotechnological applications. To gain insight into the relationship between the chemical structure, self-assembly behavior, and physicochemical properties of polypeptoids, many efforts have been made using thermal analysis, microscopy, scattering, and spectroscopic techniques. In this review, we summarize recent experimental investigations that have focused on the hierarchical self-assembly and phase behavior of polypeptoids in bulk, thin film, and solution states, highlighting the use of advanced characterization tools such as in situ microscopy and scattering techniques. These methods enable researchers to unravel multiscale structural features and assembly processes of polypeptoids over a wide range of length and time scales, thereby providing new insights into the structure-property relationship of these protein-mimetic materials.

Curvature sensing as an emergent property of multiscale assembly of septins

The ability of cells to sense and communicate their shape is central to many of their functions. Much is known about how cells generate complex shapes, yet how they sense and respond to geometric cues remains poorly understood. Septins are GTP-binding proteins that localize to sites of micrometer-scale membrane curvature. Assembly of septins is a multistep and multiscale process, but it is unknown how these discrete steps lead to curvature sensing. Here, we experimentally examine the time-dependent binding of septins at different curvatures and septin bulk concentrations. These experiments unexpectedly indicated that septins' curvature preference is not absolute but rather is sensitive to the combinations of membrane curvatures present in a reaction, suggesting that there is competition between different curvatures for septin binding. To understand the physical underpinning of this result, we developed a kinetic model that connects septins' self-assembly and curvature-sensing properties. Our experimental and modeling results are consistent with curvature-sensitive assembly being driven by cooperative associations of septin oligomers in solution with the bound septins. When combined, the work indicates that septin curvature sensing is an emergent property of the multistep, multiscale assembly of membrane-bound septins. As a result, curvature preference is not absolute and can be modulated by changing the physicochemical and geometric parameters involved in septin assembly, including bulk concentration, and the available membrane curvatures. While much geometry-sensitive assembly in biology is thought to be guided by intrinsic material properties of molecules, this is an important example of how curvature sensing can arise from multiscale assembly of polymers.

Multiscale assembly of polyoxometalates: From clusters to materials

Polyoxometalates (POMs) have drawn broad and intense interest due to their unique structure-dependent properties. The assembly of POM molecules into nanoarchitectures and superstructures can bridge the gap between micro-molecule and bulk POM materials and integrate the merits of molecule and materials that are widely used in catalysis, energy conversion, electronics, and bioapplications. The synthetic methodologies and applications of multiscale POM assemblies have been widely studied. In this review, we survey the POM-based multiscale assembly focusing on two aspects: the strategies for multiscale assembly of POMs and the emerging applications of POM assemblies. For the multiscale assembly, we focus on the methods of POMs assembly including templated synthesis and self- and co-assembly of POMs into nanoarchitectures and superstructures. For the applications, we review the applications of POM assemblies in energy, catalysis, and functional materials. Finally, we present the prospects for the future synthetic design and applications of POM assemblies.

Highly effective and tunable microwave absorber integrating multiscale attenuation behaviours derived from prussian blue analogue/graphene oxide aerogel

Tunable and efficient absorption of graphene-based microwave absorbers are essential on the realms of electromagnetic compatibility and protection in various application scenarios. However, challenges arise owing to their limited microwave attenuation behaviors. Herein, CoNiFe Prussian blue analogue (PBA)-derived magnetic alloy@carbon nanocubes anchored on N-doped reduced graphene oxide (rGO) aerogels were achieved via CoNiFe-PBA nanocubes assisting assembly of GO and subsequent thermal annealing approach. Such three-dimensional (3D) graphene-based macroscopic architecture integrates multiple attenuation behaviours occurred across multiple length scales. Attributed to the synergy of multiple scattering, conduction loss, multiple heterogeneous interface and dipolar polarizations, and magnetic loss, the optimized CoNiFe-PBA/GO aerogel derivative simultaneously exhibits strong reflection loss and wide effective bandwidth with an ultralow filling content (1.1 wt%) at both X band (−66.01 dB and 5.2 GHz at 3.2 mm) and Ku band (−66.23 dB and 6.6 GHz at 2.6 mm). Multiscale assembly strategy of graphene-based electromagnetic functional materials from molecular level to macroscale proposed and demonstrated by this work shows promise for exploring tunable and efficient microwave absorbers.

Mesoporous LDH Metastructure from Multiscale Assembly of Defective Nanodomains by Laser Shock for Oxygen Evolution Reaction.

Laser is a powerful tool for the synthesis of nanomaterials. The intensive laser pulses delivered to materials within nanoseconds allow the formation of novel structures that are inaccessible for conventional methods. Layered double hydroxide (LDH) nanostructures with high porosity, suitable dopants, and rich defects are desirable for catalysts, however, tremendously difficult in a one-pot synthesis. Here it is found that confined laser shock in solvent leads to the formation of nanoreactors which guide the assembly of multiscale LDH building units, larger nanosheets as frame and smaller nanodomains as building blocks. These nanodomains have rich vacancy defects and are interlocked in a high packed density of 1013 cm-2 , leaving rich mesopores across the nanosheets and coral-like morphology. Like the natural coral reef that has multiscale structure to accommodate different marine organisms, the coral-like LDH metastructure provides large surface area and rich active sites for the interaction with guest molecules. Benefiting from the multiscale porous structure and rational dopant, this LDH catalyst exhibits a low overpotential of 220mV at 10mAcm-2 for oxygen evolution reaction (OER), standing as one of the best LDH catalysts to date.

Constitutionally Selective Dynamic Covalent Nanoparticle Assembly.

The future of materials chemistry will be defined by our ability to precisely arrange components that have considerably larger dimensions and more complex compositions than conventional molecular or macromolecular building blocks. However, exerting structural and constitutional control in the assembly of nanoscale entities presents a considerable challenge. Dynamic covalent nanoparticles are emerging as an attractive category of reaction-enabled solution-processable nanosized building block through which the rational principles of molecular synthetic chemistry can be extended into the nanoscale. From a mixture of two hydrazone-based dynamic covalent nanoparticles with complementary reactivity, specific molecular instructions trigger selective assembly of intimately mixed heteromaterial (Au–Pd) aggregates or materials highly enriched in either one of the two core materials. In much the same way as complementary reactivity is exploited in synthetic molecular chemistry, chemospecific nanoparticle-bound reactions dictate building block connectivity; meanwhile, kinetic regioselectivity on the nanoscale regulates the detailed composition of the materials produced. Selectivity, and hence aggregate composition, is sensitive to several system parameters. By characterizing the nanoparticle-bound reactions in isolation, kinetic models of the multiscale assembly network can be constructed. Despite ignoring heterogeneous physical processes such as aggregation and precipitation, these simple kinetic models successfully link the underlying molecular events with the nanoscale assembly outcome, guiding rational optimization to maximize selectivity for each of the three assembly pathways. With such predictive construction strategies, we can anticipate that reaction-enabled nanoparticles can become fully incorporated in the lexicon of synthetic chemistry, ultimately establishing a synthetic science that manipulates molecular and nanoscale components with equal proficiency.

A programmable multiscale assembly strategy of carbon nanotubes for honeycomb-like networks

In order to meet the growing demand for high performance flexible transparent conductive electrode, starting from its hierarchical structure, a programmable multiscale assembly strategy of CNTs for honeycomb-like networks is proposed to hope to improve its performance. The analysis shows that the self-assembly method can realize the CNTs assembly of nonlinear hexagonal structure by constructing the pattern of SAMs. In this paper, a molecular dynamics model at atomic level is established for studying the self-assembly behavior to analyze its mechanism and the influencing factors of the CNTs distribution morphology. Then the process procedures are investigated to prepare multiscale honeycomb-like CNTs networks with size programmable on functionalized SiO2 substrate, while the accuracy of the molecular dynamics model is confirmed. Finally, the conductivity, transparency and transferability of the honeycomb-like CNTs networks are exploited and proved to be suitable for flexible conductive electrode with higher transparency than the CNTs film. This paper paves the way for the study of properties programmable related to the structure of CNTs assembly. Future work towards scalable and stable preparation of honeycomb-like CNTs networks will further validate them as a promising alternative to the traditional CNTs transparent conductive electrode and continue to make efforts in the field of photovoltaic and electrical sensing.

A Review on Graphene‐Based Electromagnetic Functional Materials: Electromagnetic Wave Shielding and Absorption

AbstractElectromagnetic (EM) functional materials play an increasingly important role in solving EM wave pollution in both modern military and civil fields. Graphene‐based materials are the most promising candidates in the applications of EM wave shielding and absorption owing to their remarkable structures and enhanced EM properties. Designing graphene‐based materials with elaborately controlled microstructures and optimized EM properties can effectively improve EM energy attenuation and conversion. Herein, the study begins with the EM attenuation mechanism, and multiscale design strategies of graphene‐based EM functional materials are outlined, including molecular‐scale, micro/nanoscale structure, macroscale structure, and integration of multiscale assembly design strategies. Applications in the EM wave shielding and absorption fields are reviewed, focusing on the latest advances in graphene‐based assemblies such as films, fabrics, and composites. Finally, the current challenges and future directions in this fast‐growing field are predicted.

Robust, Healable, Self-Locomotive Integrated Robots Enabled by Noncovalent Assembled Gradient Nanostructure.

Integration, being lightweight, and intelligence are important orientations for the future advancement of soft robots. However, existing soft robots are generally hydrogels or silicone rubber, which are inherently mechanically inferior and easily damaged and difficult to integrate functions. Here, inspired by nacre, an elastomer actuator with sulfonated graphene-based gradient nanostructures is constructed via supramolecular multiscale assembly. The resulting nanocomposite possesses an ultrahigh toughness of 141.19 MJ/m3 and high room-temperature self-healing efficiency (89%). The proof-of-concept robot is demonstrated to emphasize its maximum swimming speed of 2.67 body length per second, whose speed is comparable to that of plankton, representing the outperformance of most artificial soft robots. Furthermore, the robot can stably absorb pollutants and recover its robustness and functionality even when damaged. This study breaks the mutual exclusivity of functional execution and fast locomotions, and we anticipate that our nanostructural design will offer an effective extended path to other integrated robots that required multifunction integration.