2D MXene Research Articles

Tailoring surface terminals on MXene enables high-efficiency electromagnetic absorption

MXene (Ti3C2Tx) is an important category of two-dimensional (2D) materials due to its distinctive metallic conductivity and adjustable surface chemistry. The exceptional benefits of heterointerface and defects or viods, combined with the distinct electromagnetic (EM) properties, inject boundless potential into the advancement of MXene-based absorbers for EM absorbing materials. However, conventional synthetic methods depend on chemical etching of MAX powders (Ti3AlC2) using hazardous HF or similar substances, resulting in MXene sheets with fluorine termination and limited stability in colloidal dispersions under ambient conditions. Herein, varied synthetic routes were proposed to prepare MXenes with different terminal groups by the fluoride-based salts, fluoride-free molten salts, and alkali etching. 2D MXene nanosheets with abundant surface groups are excellent EM absorbing materials, and the MXene etched by the Lewis acid CuCl2 delivered remarkable reflection loss (RL) value of −47.56 dB at 2.5 mm and broad bandwidth of 4.8 GHz due to promoted interfacial polarization. By conducting a thorough examination of the structural changes in MXenes, this study aims to propose a viable method for delaminating single-layer MXene and elucidate the EM absorption mechanisms.

Temperature driven pseudocapactive performance of WO3/MXene nanocomposite for asymmetric aqueous supercapacitors

The WO3 nanostructured materials are widely used as a pseudocapacitive charge storage electrodes. However it is restricted by poor cyclic stability. To overcome it, hybrid nanocomposites materialization of WO3 with fascinating 2D MXene is an excellent strategy. Though both materials consumes acid based electrolytes and possesses layered structures, WO3 protects MXene from self-restacking and/or aggregation of their adjacent layers owing to its strong van-der Waals interaction. Moreover layered structure of MXene offers synergistic action of various metal elements, fast diffusion of ions, increase the voltage window and cycle life. Herein we report hybrid nanocomposite of orthorhombic WO3 nanoplates with 2D MXene nanoflakes prepared by a single-step hydrothermal method. The electrochemical investigations exhibits the specific capacitances of 21 F g−1 (MXene), 112 F g−1 (WO3), and 290 F g−1 (WO3/MXene-20) at 0.5 A g−1 in 1 M H2SO4 aqueous electrolyte. Furthermore temperature dependent investigation of a hybrid nanocomposite (WO3/MXene-20) demonstrates consistent enhancement in the specific capacitance with the increasing temperature and a maximum capacitance of 376 F g−1 at 0.5 A g−1 is achieved at 50 °C. Eventually an asymmetric aqueous supercapacitor (AASC) fabricated using hybrid nanocomposite (WO3/MXene-20) demonstrates an outstanding cyclic stability up to 20,000 cycles at 5 A g−1 upholding 72 % capacitance retention and 73 % coulombic efficiency. The exceptional cyclic stability of the AASC configuration emphasizes the prospective of WO3/MXene hybrid nanocomposites for durable energy storage applications.

Environment-friendly synthesis of Ti3C2TX MXene by etching and galvanic reactions for Al removal of Ti3AlC2 MAX

Although MXene is acknowledged as next generation two-dimensional (2D) nanomaterials, in general, MXene has been obtained by using hazardous and corrosive etching agents such as HF and HCl. Therefore, in the present study, we report on the environment-friendly synthesis of 2D Ti3C2TX MXene using weak acid H3PO4 as etchant. We compare the Al etching capacity of H3PO4 paired with various metal fluorides (LiF, ZnF2, CuF2) to in-situ form HF. Out of all metal fluoride candidates, CuF2 is the most effective in the etching of Ti3AlC2 MAX not only due to the reaction of F− with Al but also the galvanic replacement of Cu2+ with Al. As a result, Ti3AlC2 MAX is mostly etched using H3PO4/CuF2 within only 4 h reaction and is completely etched in 12 h reaction. After etching, the Cu intercalated between MXene layers is extracted using maleic acid forming a Cu-maleic acid complex to produce exfoliated 2D MXene nanosheets. The exfoliated MXene contains mainly −F, −O, –OH surface terminations and a small portion of −PO4, exhibiting the good aqueous dispersibility.

Recent Advances in Non-Ti MXenes: Synthesis, Properties, and Novel Applications.

One of the most fascinating 2D nanomaterials (NMs) ever found is various members of MXene family. Among them, the titanium-based MXenes, with more than 70% of publication-related investigations, are comparatively well studied, producing fundamental foundation for the 2D MXene family members with flexible properties, familiar with a variety of advanced novel technological applications. Nonetheless, there are still more candidates among transitional metals (TMs) that can function as MXene NMs in ways that go well beyond those that are now recognized. Systematized details of the preparations, characteristics, limitations, significant discoveries, and uses of the novel M-based MXenes (M-MXenes), where M stands for non-Ti TMs (M=Sc, V, Cr, Y, Zr, Nb, Mo, Hf, Ta, W, and Lu), are given. The exceptional qualities of the 2D non-Ti MXene outperform standard Ti-MXene in several applications. There is many advancement in top-down as well as bottom-up production of MXenes family members, which allows for exact control of the M-characteristics MXene NMs to contain cutting-edge applications. This study offers a systematic evaluation of existing research, covering everything in producing complex M-MXenes from primary limitations to the characterization and selection of their applications in accordance with their novel features. The development of double metal combinations, extension of additional metal candidates beyond group-(III-VI)B family, and subsequent development of the 2D TM carbide/TMs nitride/TM carbonitrides to 2D metal boride family are also included in this overview. The possibilities and further recommendations for the way of non-Ti MXene NMs are in the synthesis of NMs will discuss in detail in this critical evaluation.

Hierarchical heterostructures of MXene and mesoporous hollow carbon sphere for improved ion accessibility and rate performance

The development of electrode materials with a hierarchically porous structure and good electrical connection is key to improving the charging-discharging rate and energy density of supercapacitors. However, the restacking issue of two-dimensional nanomaterials, such as MXene, seriously hinders the diffusion of electrolyte ions. Different from the extensively used sacrificing template method, a hierarchical heterostructure of electrically conducting mesoporous hollow carbon spheres (MHCS) and MXene composite electrode is designed and achieved through simple vacuum filtration without further template removing procedures. This direct preparation strategy not only effectively improves the specific surface area of the electrode but also enhances the abundant surface pores and good conductivity of MHCS, improving the penetration of the electrolyte solution and shortening the ion transport path, leading to a pronounced improvement in specific capacitance and rate performance of the electrodes. Additionally, the influence of sheath thickness of MHCSs on ion transfer rate is deeply discussed. The introduction of carbon nanotubes (CNTs) further improves conductivity and stability while maintaining good flexibility. Consequently, the MXene/MHCS/CNT film delivers a high specific capacitance (395F g−1 at 2 mV s−1), outstanding rate performance (70.9 % at 1000 mV s−1), and excellent cycling stability (98.3 % capacity retention after 10,000 cycles). Furthermore, the assembled symmetric supercapacitor provides a maximum energy density of 14.48 Wh kg−1. This work provides a quick and effective approach for constructing high performance 3D MXene architectures for fast ion transfer electrodes.

MXene Sediment-Based Poly(vinyl alcohol)/Sodium Alginate Aerogel Evaporator with Vertically Aligned Channels for Highly Efficient Solar Steam Generation

HighlightsMXene sediments is innovatively used as photothermal material for seawater desalination.Inspired by the natural wood transpiration process, a 3D MXene sediment-based aerogel with vertically aligned channels is innovatively prepared as solar evaporator.With unique structure and composition, excellent photothermal conversion efficiency, evaporation rate, salt resistance, and resistance to biological/oil/special environments are achieved in practical desalination.

The impact of surface functional groups on MXene anode protective layer in aqueous zinc-ion batteries: Understanding the mechanism

The development of energy storage has seen a significant increase in the use of aqueous zinc-ion batteries (AZIBs) with intrinsic safety, which have become an important choice for new high-security energy storage. However, the dendrite growth and hydrogen evolution reaction (HER) on Zn anodes present a significant challenge to the commercialisation of AZIBs. The stability of Zn anodes can be effectively improved by using an anodic interfacial protective layer. The novel two-dimensional (2D) MXene material is capable of effectively inhibiting zinc dendrite growth and the HER reaction when employed as a protective layer for AZIBs anodes due to its readily adjustable properties. The surface functional groups of MXene exhibit different electrochemical properties in different electrolytes, which affects the realization of the protective function. The current understanding of the influence of these surface functional groups on the monolayer MXene as an anodic protective layer for AZIBs is incomplete. A combination of density functional theory calculations and molecular dynamics simulations was employed to investigate the electronic properties, adsorption energies for Zn2+ and H2O, free energies for HER, Zn2+ diffusion energy barriers, Zn2+ diffusion coefficients, and coordination numbers of Zn2+ with water molecules of monolayer MXene (Mo2CTx) with nine different surface functional groups were investigated. The mechanism of the impact of surface functional groups on monolayer Mo2CTx as an anodic protective layer for AZIBs was elucidated. This study will provide guidance for the extensive use of MXene materials in AZIBs to effectively enhance the anode stability and prolong the battery operation life.

Thickness‐ and Wavelength‐Dependent Nonlinear Optical Absorption in 2D Layered MXene Films

As a rapidly expanding family of 2D materials, MXenes have recently gained considerable attention. Herein, by developing a coating method that enables transfer‐free and layer‐by‐layer film coating, the nonlinear optical absorption (NOA) of Ti3C2Tx MXene films is investigated. Using the Z‐scan technique, the NOA of the MXene films is characterized at ≈800 nm. The results show that there is a strong and layer‐dependent NOA behavior, transitioning from reverse saturable absorption (RSA) to saturable absorption (SA) as the layer number increases from 5 to 30. Notably, the nonlinear absorption coefficient β changes significantly from ≈7.13 × 102 cm GW−1 to ≈−2.69 × 102 cm GW−1 within this range. The power‐dependent NOA of the MXene films is also characterized, and a decreasing trend in β is observed for increasing laser intensity. Finally, the NOA of 2D MXene films at ≈1550 nm is characterized by integrating them onto silicon nitride waveguides, where an SA behavior is observed for the films including 5 and 10 layers of MXene, in contrast to the RSA observed at ≈800 nm. These results reveal intriguing nonlinear optical properties of 2D MXene films, highlighting their versatility and potential for implementing high‐performance nonlinear photonic devices.

Multi-Scale MXene/Silver Nanowire Composite Foams with Double Conductive Networks for Multifunctional Integration.

With the onset of the 5G era, wearable flexible electronic devices have developed rapidly and gradually entered the daily life of people. However, the vast majority of research focuses on the integration of functions and performance improvement, while ignoring electromagnetic hazards caused by devices. Herein, the 3D double conductive networks are constructed through a repetitive vacuum-assisted dip-coating technique to decorate the 2D MXene and 1D silver nanowires on the melamine foam. Benefiting from the unique porous structure and multi-scale interconnected frame, the resultant composite foam exhibited high electrical conductivity, low density, superb electromagnetic interference shielding (48.32dB), and Joule heating performance (up to 90.8°C under 0.8V). Furthermore, a single-electrode triboelectric nanogenerator (TENG) with powerful energy harvesting capability is assembled by combining the composite foam with an ultra-thin Ecoflex film and a polyvinylidene fluoride film. Simultaneously, the foam-based TENG can also be considered a reliable wearable sensor for monitoring activity patterns in different parts of the human body. The versatility and scalable manufacturing of high-performance composite foams will provide new design ideas for the development of next-generation flexible wearable devices.

Non‐Ti (M2X and M3X2) MXenes for Energy Storage/Conversion

AbstractMXenes, with a particular emphasis on Ti3C2 (M3X2) have been extensively studied and established as the foundational material for 2D MXenes. However, the exploration of other transitional metals as 2D MXenes holds great promise, offering applications beyond the existing knowledge. Non‐Ti (M2X and M3X2) MXenes have garnered attention due to their distinctive properties. This review article focuses on explaining the potential and challenges of non‐Ti (M2X and M3X2) MXenes in energy storage and conversion systems, specifically in the domains of supercapacitors, batteries (Li‐ion and Li‐S), oxygen evolution reaction (OER), hydrogen evolution reaction (HER), and oxygen reduction reaction (ORR). By providing a comprehensive overview of the current progress and addressing the associated challenges, this review offers valuable insights into the future prospects of not only non‐Ti (M2X and M3X2) MXenes but also other MXenes for energy storage and conversion. The findings presented herein pave the way for further research and multifaceted applications of these MXenes across various fields.

3D vertical ultra-sodiophilic leaf-vein-like MXene/Sn@CNF array of structured sodium enabling high-rate and long-life sodium metal batteries

Uncontrolled Na dendrite growth and infinite volume change during cycling have greatly impeded the practical application of Na metal anode for high-energy-density batteries. To address these two issues simultaneously, a 3D vertical ultra-sodiophilic leaf-vein-like MXene/Sn@CNF array (VL-MXene/Sn@CNF) aerogel, integrated by 1D Sn@CNF and 2D MXene, was prepared by an ingenious hydrogen bonding self-assembly and unidirectional ice template method. The low-tortuosity and ultra-sodiophilic vertical array facilitates uniform and rapid Na+ transport along the ordered interspaces, achieving a negligible nucleation overpotential of 1.0 mV. Furthermore, experimental results and theoretical calculations revealed a unique bidirectional growth mode of Na, in which vertical leaf-vein-like lamellae and bridging fibers guided Na to be densely deposited along the vertical and horizontal directions, respectively. Benefitting from the ultra-sodiophilic vertical array of structured Na, the designed material exhibits an endurance of 1000 cycles for asymmetric cell at 3.0 mA cm−2 and 3.0 mAh cm−2, and the symmetrical cell delivers an ultra-long lifespan of 6000 h at 1.0 mA cm−2 and 3.0 mAh cm−2 with a high depth of discharge up to 50 %. Remarkably, at the high current of 15 C, the full cell based on NaTi2(PO4)3 cathode and Na@VL-MXene/Sn@CNF anode can deliver a reversible capacity of 88.94 mAh g−1 after 9200 cycles with an ultralow 0.0016 % capacity decay per cycle, which represents the most impressive full cell performance so far.

Preparation and properties of two-dimensional Ti2CT x MXene based on electroetching method

The continuous advancements in wearable electronics have drawn significant attention toward 2D MXenes materials for energy storage owing to their abundant availability, adaptability, and distinctive physicochemical properties. Two unresolved concerns currently revolve around environmental pollution by F-containing etching and finite kinetics caused because of re-stacking of nanosheets. In this study, Al was electrochemically etched from porous Ti2AlC electrodes without the use of fluorine, through a selective electrochemical etching process in dilute hydrochloric acid. Subsequently, Ti2CT x MXene was vertically grown on carbon fiber (CF) substrates. The resulting Ti2CT x @CF electrodes are lightweight, thin, and flexible, exhibiting a surface capacitance of 330 mF cm−2 at a constant current density of 1 mA cm−2 after 2000 cycles. They display a surface capacitance retention of 96.16% and a high energy density of 45.3 μWh cm−2 at a power density of 0.497 mW cm−2. These metrics underscore the Ti2CT x @CF electrode’s commendable multifunctionality, electrochemical performance, ion transport efficiency, and charge storage capacity. Moreover, a flexible energy storage electrode material with a high area capacity was developed by combining Ti2CT x MXene nanosheets, possessing a large specific surface area, with a flexible carbon fabric substrate.

Ultrastable Organic Anode Enabled by Electrochemically Active MXene Binder toward Advanced Potassium Ion Storage.

Conjugated carbonyl compounds are regarded as promising organic anode materials for potassium ion batteries (PIBs) due to their rich redox sites, excellent reversibility, and structural tunability, but their low electrical conductivity and severe solubility in organic electrolytes have substantially restricted their practical application. Herein, 2D MXene is utilized as an electrochemically active binder to fabricate perylene-3,4,9,10-tetracarboxylic dianhydride (PTCDA) electrodes for high-performance PIBs. MXene, coupled with Super-P particles, served as a binder and conductive matrix to facilitate rapid ion and electron transport, restrain the solubility of PTCDA, promote potassium adsorption, and alleviate the volume expansion of PTCDA during potassiation. Consequently, the PTCDA electrode bonded by the MXene/Super-P system delivers excellent potassium storage performance in terms of a high capacity of 462 mAh g-1 at 50 mA g-1, superior rate capability of 116.3 mAh g-1 at 2000 mA g-1, and stable cycle performance over 3000 cycles with a low capacity decay rate of ∼0.0033% per cycle. When configured with the PTCDA@450 cathode, an all-PTCDA potassium ion full cell delivers a maximum energy density of 179.5 Wh kg-1, indicating the superiority of MXene as an electrochemically active binder to promote the practical application of organic anodes for PIBs.

Two-dimensional MXene Nanomaterials: Preparation, Structure Modulation and the Applications in Electrochemical Energy Storage.

MXenes have attracted intensive attention owing to their unique twodimensional (2D) layered structure, high specific surface area, excellent conductivity, superior surface hydrophilicity, and chemical stability. In recent years, selective etching of the A element layers from MAX phases by fluorine-containing etchants (HF, LiF-HCl, etc) is a common method to prepare multilayered MXene nanomaterials (NMs) with plentiful surface terminations. At present, many studies have been reported on the use of fluorine-free etchants (NaOH, ZnCl2, etc) to etch MAX phases. The properties of MXene NMs are dependent on their structures. The purpose of this review is to focus on a comprehensive and systematical survey on the preparation, structure modulation, and applications of MXene NMs in electrochemical energy storage devices, including supercapacitors, lithium-ion battery, sodium-ion battery, potassium-ion battery, and aluminum-ion battery. Extensive information related to the preparation and applications of 2D MXene NMs for electrochemical energy storage and their associated patents were collected. This review highlights the recently reported 2D MXene NMs which are used in supercapacitor and various metal ion. It is found that the preparation methods have great impacts on the layer spacing and surface terminations of MXenes, consequently affecting their performance. Hence, this paper summarizes the research progress of the preparation strategies, layer spacing and surface termination modulation of MXene NMs. The applications of 2D MXene NMs in electrochemical energy storage are outlined. The forward-looking challenges and prospects for the development of MXenes are also proposed.

Multifunction integration within magnetic CNT-bridged MXene/CoNi based phase change materials

Developing advanced nanocomposite phase change materials (PCMs) integrating zero-energy thermal management, microwave absorption, photothermal therapy and electrical signal detection can promote the leapfrog development of flexible wearable electronic devices. For this goal, we propose a multidimensional collaborative strategy combining two-dimensional (2D) MXene nanosheets with metal-organic framework-derived one-dimensional (1D) carbon nanotubes (CNTs) and zero-dimensional (0D) metal nanoparticles. After encapsulating paraffin wax (PW) in three-dimensional (3D) networked multidimensional MXene/CoNi–C, the resulting composite PCMs exhibit excellent thermal energy storage capacity and long-term thermally reliable stability. Benefiting from the synergistically enhanced photothermal effects of CNTs, Co/Ni nanoparticles and MXene, PW@MXene/CoNi–C can capture photons efficiently and transfer phonons quickly, yielding an ultrahigh photothermal conversion and storage efficiency of 97.5%. Additionally, PW@MXene/CoNi–C composite PCMs exhibit high microwave absorption with a minimum reflection loss of −49.3 ​dB at 8.03 ​GHz in heat-related electronic application scenarios. More attractively, the corresponding flexible phase change film can simultaneously achieve thermal management and electromagnetic shielding of electronic devices, as well as photothermal therapy and electrical signal detection for individuals. This functional integration design provides an important reference for developing advanced flexible multifunctional wearable materials and devices.

Calcium phosphate graphene and Ti3C2Tx MXene scaffolds with osteogenic and antibacterial properties.

Bioactive degradable scaffolds that facilitate bone healing while fighting off initial bacterial infection have the potential to change established strategies of dealing with traumatic bone injuries. To achieve this a composite material made from calcium phosphate graphene (CaPG), and MXene was synthesized. CaPG was created by functionalizing graphene oxide with phosphate groups in the presence of CaBr with a Lewis acid catalyst. Through this transformation, Ca2+ and PO4 3- inducerons are released as the material degrades thereby aiding in the process of osteogenesis. The 2D MXene sheets, which have shown to have antibacterial properties, were made by etching the Al from a layered Ti3AlC2 (MAX phase) using HF. The hot-pressed scaffolds made of these materials were designed to combat the possibility of infection during initial surgery and failure of osteogenesis to occur. These two failure modes account for a large percentage of issues that can arise during the treatment of traumatic bone injuries. These scaffolds were able to retain induceron-eluting properties in various weight percentages and bring about osteogenesis with CaPG alone and 2 wt% MXene scaffolds demonstrating increased osteogenic activity as compared to no treatment. Additionally, added MXene provided antibacterial properties that could be seen at as little as 2 wt%. This CaPG and MXene composite provides a possible avenue for developing osteogenic, antibacterial materials for treating bone injuries.

Advanced Insights on MXenes: Categories, Properties, Synthesis, and Applications in Alkali Metal Ion Batteries.

The development and optimization of promising anode material for next-generation alkali metal ion batteries are significant for clean energy evolution. 2D MXenes have drawn extensive attention in electrochemical energy storage applications, due to their multiple advantages including excellent conductivity, robust mechanical properties, hydrophilicity of its functional terminations, and outstanding electrochemical storage capability. In this review, the categories, properties, and synthesis methods of MXenes are first outlined. Furthermore, the latest research and progress of MXenes and their composites in alkali metal ion storage are also summarized comprehensively. A special emphasis is placed on MXenes and their hybrids, ranging from material design and fabrication to fundamental understanding of the alkali ion storage mechanisms to battery performance optimization strategies. Lastly, the challenges and personal perspectives of the future research of MXenes and their composites for energy storage are presented.

Improved Surface-Enhanced Raman Scattering Performance of 2D Ti3C2Tx MXene Embedded in PVDF Film Enabled by Photoinduction and Electric Field Modulation.

In this study, we introduce a synergistic approach to enhance the surface-enhanced Raman scattering (SERS) signal in two-dimensional (2D) MXene through photo-irradiation and electric field modulation. Our methodology involves the integration of 2D Ti3C2Tx MXene with piezoelectric polyvinylidene fluoride (PVDF) polymer, resulting in the creation of a free-standing, flexible composite film. On this composite film, a thin layer of Au was deposited. Our flexible substrate was able to sense methylene blue (MB), crystal violet (CV), 4-aminothiophenol (ATP), and melamine. The SERS substrate exhibits low detection limit of 10-8 M MB with a 6.7 × 106 enhancement factor (EF). The SERS substrate enables picomolar (pM) detection sensitivity for CV molecules with an EF of 9.2 × 109. Furthermore, the introduction of photo-irradiation leads to an additional ∼3.5-fold enhancement in the SERS signal, which is attributed to the altered work function and defects. The application of mechanical force to the piezoelectric PVDF/Ti3C2Tx film results in a ∼4.5-fold boost in SERS signal due to mechanical force-induced electrical energy. The fabrication strategy employed here for producing a flexible piezoelectric PVDF/Ti3C2Tx film holds significant promise for expanding the potential application of 2D MXene in rapid, on-site sensing scenarios.

Sodium alanate in-situ doped with Ti2C MXene with enhanced hydrogen storage properties

NaAlH4 is a reversible hydrogen storage material and has attracted great attention recently. However, the application of NaAlH4 in hydrogen storage still has great difficulties. In this study, 2D MXene Ti2C-doped NaAlH4 samples were prepared in-situ by reaction ball milling of NaH under moderate condition. TPD measurement results show that all the as-prepared samples exhibit good thermodynamic performance except for the sample doped with 1 wt% Ti2C. And DSC analysis results show that at the heating rate of 5 K/min, the first and second dehydrogenation peak temperatures of the sample doped with 7 wt% Ti2C were 127.1 °C and 150.6 °C respectively, which are 57.4 °C and 123.6 °C lower than those of pure NaAlH4 (after ball milling), respectively. Meanwhile, NaH/Al-7 wt.% Ti2C sample displays a superior kinetics behavior. Isothermal hydrogen evolution curves show that NaH/Al-7 wt.%Ti2C released 5.21 wt% H2 within 30 min at 150 °C and then absorbs 5.2 wt% H2 in 90 s at 120 °C. Even at a lower temperature of 80 °C, the sample still absorbed 4.71 wt% H2 within 60 min. In addition, almost no release capacity attenuation was observed for NaH/Al-7 wt.%Ti2C after 10 hydrogen absorption/desorption cycles. The improvement of the hydrogen storage properties can be ascribed to the high reactivity of NaAlH4 produced in situ and catalysis of lamellar Ti3+/0 species formed by the reduction of high valent Ti in Ti2C during ball milling.

Rational design of MXene/MWCNT/TOCNF film for flexible supercapacitor

Two-dimensional (2D) MXenes are widely acknowledged as highly adaptable materials for flexible supercapacitors due to their high electronic conductivity, tunable surface chemistry, structural adaptability, and excellent mechanical strength. However, pure MXene nanosheets have a tendency to stack together, which decreases the mechanical and electrochemical properties for flexible devices. Herein, inspired by the structure of modern architecture, MXene/MWCNT/2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO) radical-mediated oxidized cellulose nanofibers (TOCNFs) (MMT) composite film (MMT-X, the content of MWCNT and TOCNFs is X% of the total weight of the film) is manufactured using a simple vacuum filtration method. In MMT, two-dimensional (2D) MXene is severed as nanometer “bricks”, one-dimensional (1D) TOCNFs is used as a nanometer “mortar” between MWCNTs and MXene based on synergistic electrostatic forces and hydrogen bonding to build a three-dimensional (3D) composite structures with excellent mechanical strength. The flexible MMT-8 film is used as a supercapacitor electrode with specific capacity 856 F cm−3. Furthermore, at a volume power density of 335.5 W L−1, the assembled flexible all-solid-state supercapacitor (ASSC) could provide a volumetric energy density of 11.64 Wh L−1 with good cycle stability.