Reversible Hydrogen Bonds Research Articles

Development of a Sustainable Flexible Humidity Sensor Based on Tenebrio molitor Larvae Biomass-Derived Chitosan.

This study presents the fabrication of a sustainable flexible humidity sensor utilizing chitosan derived from mealworm biomass as the primary sensing material. The chitosan-based humidity sensor was fabricated by casting chitosan and polyvinyl alcohol (PVA) films with interdigitated copper electrodes, forming a laminate composite suitable for real-time, resistive-type humidity detection. Comprehensive characterization of the chitosan film was performed using Fourier-transform infrared (FTIR) spectroscopy, contact angle measurements, and tensile testing, which confirmed its chemical structure, wettability, and mechanical stability. The developed sensor exhibited a broad range of measurements from 6% to 97% relative humidity (RH), a high sensitivity of 2.43 kΩ/%RH, and a rapid response time of 18.22 s with a corresponding recovery time of 22.39 s. Moreover, the chitosan-based humidity sensor also demonstrated high selectivity for water vapor when tested against various volatile organic compounds (VOCs). The superior performance of the sensor is attributed to the structural properties of chitosan, particularly its ability to form reversible hydrogen bonds with water molecules. This mechanism was further elucidated through molecular dynamics simulations, revealing that the conductivity in the sensor is modulated by proton mobility, which operates via the Grotthuss mechanism under high-humidity and the packed-acid mechanism under low-humidity conditions. Additionally, the chitosan-based humidity sensor was further seamlessly integrated into an Internet of Things (IoT) framework, enabling wireless humidity monitoring and real-time data visualization on a mobile device. Comparative analysis with existing polymer-based resistive-type sensors further highlighted the superior sensing range, rapid dynamic response, and environmental sustainability of the developed sensor. This eco-friendly, biomass-derived, eco-friendly sensor shows potential for applications in environmental monitoring, smart agriculture, and industrial process control.

Large stroke radially oriented MXene composite fiber tensile artificial muscles.

Actuation is normally dramatically enhanced by introducing so much yarn fiber twist that the fiber becomes fully coiled. In contrast, we found that usefully high muscle strokes and contractile work capacities can be obtained for non-twisted MXene (Ti3C2Tx) fibers comprising MXene nanosheets that are stacked in the fiber direction. The MXene fiber artificial muscles are called MFAMs. We obtained MFAMs that have high modulus in both the radial and axial directions by spinning a solution containing MXene nanosheets dispersed in an aqueous cellulose solution. We observed a highly reversible muscle contraction of 21.0% for a temperature increase from 25° to 125°C. The tensile actuation of MFAMs mainly results from reversible hydrogen bond orientation change during heating, which decreases intra-sheet spacing. The MFAMs exhibited fast, stable actuation to multiple temperature-generating stimuli, which increases their applications in smart textiles, robotic arms, and robotic grippers.

Artificial self-powered and self-healable neuromorphic vision skin utilizing silver nanoparticle-doped ionogel photosynaptic heterostructure

Artificial skin should embody a softly functional film that is capable of self-powering, healing and sensing with neuromorphic processing. However, the pursuit of a bionic skin that combines high flexibility, self-healability, and zero-powered photosynaptic functionality remains elusive. In this study, we report a self-powered and self-healable neuromorphic vision skin, featuring silver nanoparticle-doped ionogel heterostructure as photoacceptor. The localized surface plasmon resonance induced by light in the nanoparticles triggers temperature fluctuations within the heterojunction, facilitating ion migration for visual sensing with synaptic behaviors. The abundant reversible hydrogen bonds in the ionogel endow the skin with remarkable mechanical flexibility and self-healing properties. We assembled a neuromorphic visual skin equipped with a 5 × 5 photosynapse array, capable of sensing and memorizing diverse light patterns.

Self-Healing, Electrically Conductive, Antibacterial, and Adhesive Eutectogel Containing Polymerizable Deep Eutectic Solvent for Human Motion Sensing and Wound Healing.

Flexible electronic devices such as wearable sensors are essential to advance human-machine interactions. Conductive eutectogels are promising for wearable sensors, despite their challenges in self-healing and adhesion properties. This study introduces a multifunctional eutectogel based on a novel polymerizable deep eutectic solvent (PDES) prepared by the incorporation of diallyldimethylammonium chloride (DADMAC) and glycerol in the presence of polycyclodextrin (PCD)/dopamine-grafted gelatin (Gel-DOP)/oxidized sodium alginate (OSA). The synthesized eutectogel has reversible Schiff-base bonds, hydrogen bonds, and host-guest interactions, which enable rapid self-healing upon network disruption. GPDO-15 eutectogel has significant tissue adhesion, high stretchability (419%), good ionic conductivity (0.79 mS·cm-1), and favorable antibacterial and self-healing properties. These eutectogels achieve 90% antibacterial effect, show excellent biocompatibility, and can be used as sensors to monitor human activities with strong stability and durability. The in vivo studies indicate that the eutectogels can improve the wound healing process which makes them an effective option for biological dressings.

Multistimuli-Responsive Soft Actuators with Controllable Bionic Motions.

Soft actuators with biomimetic self-regulatory intelligence have garnered significant scientific interest due to their potential applications in robotics and advanced functional devices. We present a multistimuli-responsive actuator made from a carbon nitride/carbon nanotube (CN/CNTs) composite film. This film features a molecular switch based on reversible hydrogen bonds, whose asymmetric distribution endows the film with the ability to absorb water unevenly and convert molecular motion into macroscopic movement. By incorporating carboxylated CNTs, the film demonstrates improved mechanical properties and actuation performance. Under ambient humidity stimuli, the actuator can autonomously generate walking and tumbling motions. The CN/CNTs composite film's actuating behaviors are programmable, enabling diverse deformation modes and complex biomimetic movements. Additionally, the film exhibits excellent photothermal conversion efficiency (74.10 °C/s), allowing for temperature and light-responsive actuation, which can be remotely controlled in real time. These features have enabled the creation of soft robots capable of complex biomimetic actions such as jumping, directional movement, and transporting objects. This research broadens the potential applications of CN-based actuators and paves the way for the development of intelligent soft robots.

Effect of lubricant loading in slippery liquid-infused surface for persistent anti-icing performance

Due to the vast applications in biomedical materials and aerospace industry, smart slippery liquid-infused porous surfaces (SLIPSs) have attracted remarkable attention. However, there are still challenges in the fabrication of durable SLIPS. In this work, based on linear polyurea and silicone oil, a series of durable anti-icing surface were fabricated. Based on the long-lasting secretion of lubricant, the ice adhesion strength of 60-PUa was 2.7 ± 0.5 kPa and could remain below 10 kPa even after 30 icing-deicing cycles. And the icing delay time of 60-PUa could be extended up to 870 s at a temperature of −15 °C. The introduction of large numbers of reversible hydrogen bonds in the system and silicone oil made it possible to achieve high self-healing efficiency under natural conditions. The coating system not only improved the ice removal ability, but also had excellent water-sliding properties, the droplet could slide under its own weight on 60-PUa at a tilt angle of 4.7°. This work provides an easy way to fabricate multi-functional SLIPS with durability.

Facile synthesis of high-performance and self-healing polyurethane-urea nanocomposites reinforced with graphene

In this study, a facile method was employed to synthesize strong, yet highly elastic polyurethane-urea (PUU) with typical characteristics and 94 ​% optical transmittance. Graphene platelets (GNPs) were prepared and modified via a scalable and eco-friendly mechanochemical approach. The produced GNPs is at 1.6-nm thickness with high electrical conductivity of ∼950 ​S/m. The structure-property relations of PUU/GNP nanocomposites were comprehensively investigated through morphology and mechanical properties measurements. The strong interface and high-density hydrogen bonds between modified GNPs (M-GNPs) and PUU significantly enhanced the mechanical properties of the PUU nanocomposite. The PUU composite showed 66.7 ​% and 36.2 ​% increments in tensile and impact strengths, respectively, at 0.2 ​wt% M-GNPs. The reversible hydrogen bond between M-GNPs and PUU endowed the nanocomposite with self-healing properties achieving 97.8 ​% healing efficiency of the strength after 5 ​h at 120 ​°C. This study demonstrates the importance of surface modification and provides a simple yet robust approach for preparing high-performance and functional PUU/graphene composites.

Bio-Based Polyurethane-Urea with Self-Healing and Closed-Loop Recyclability Synthesized from Renewable Carbon Dioxide and Vanillin.

Developing recyclable and self-healing non-isocyanate polyurethane (NIPU) from renewable resources to replace traditional petroleum-based polyurethane (PU) is crucial for advancing green chemistry and sustainable development. Herein, a series of innovative cross-linked Poly(hydroxyurethane-urea)s (PHUUs) were prepared using renewable carbon dioxide (CO2) and vanillin, which displayed excellent thermal stability properties and solvent resistance. These PHUUs were constructed through the introduction of reversible hydrogen and imine bonds into cross-linked polymer networks, resulting in the cross-linked PHUUs exhibiting thermoplastic-like reprocessability, self healing, and closed-loop recyclability. Notably, the results indicated that the VL-TTD*-50 with remarkable hot-pressed remolding efficiency (nearly 98.0%) and self-healing efficiency (exceeding 95.0%) of tensile strength at 60 °C. Furthermore, they can be degraded in the 1M HCl and THF (v:v = 2:8) solution at room temperature, followed by regeneration without altering their original chemical structure and mechanical properties. This study presents a novel strategy for preparing cross-linked PHUUs with self-healing and closed-loop recyclability from renewable resources as sustainable alternatives for traditional petroleum-based PUs.

Self‐healing, low oil leakage and recyclable thermally conductive Al2O3/boron nitride@siloxane composites based on reversible dynamic network

AbstractIn order to overcome the commercialized silicone‐based thermal interface materials' issues such as oil leakage and mechanical damage, we developed a thermoset silicone rubber matrix (SR) achieved through the condensation reaction of hydroxyl silicone oil and tetraethyl silicate. Additionally, we constructed a self‐healing and recyclable silicone rubber matrix (SCNR) by incorporating heat reversible ionic and hydrogen bonds between carboxyl and amino functionalized polydimethylsiloxane. Finally, the flexible, low oil leakage, self‐healing, and recyclable composites Al2O3/BN@SR/SCNR was prepared by adjusting the ratio of SR/SCNR and the spherical alumina and boron nitride (BN) fillers. The results indicated that with SR/SCNR mass ratio of 1/0.075 and filler content of 70 wt%, the thermal conductivity of the composite reaches 1.866 W m−1 K−1, 646% increasing over the SR/SCNR matrix. The self‐healing efficiency reaches 97% and the thermal conductivity remains essentially unchanged after being recycled for three times. The composites can be bent and twisted multiple times and still return to their original shape. Notably, the oil leakage of the Al2O3/BN@SR/SCNR composites is significantly lower than that of additive silicone composites. Therefore, the recyclable thermal conductivity composite developed in this study provides a promising solution for improving the durability of heat dissipation materials in electronic devices.

Proton Hydrogel-Based Supercapacitors with Rapid Low-Temperature Self-Healing Properties.

Hydrogel-based supercapacitors are an up-and-coming candidate for safe and portable energy storage. However, it is challenging for hydrogel electrolytes to achieve high conductivity and rapid self-healing at subzero temperatures because the movements of polymer chains and the reconstruction capability of broken dynamic bonds are limited. Herein, a highly conductive proton polyacrylamide-phytic acid (PAAm-PA) hydrogel electrolyte with rapid and autonomous self-healing ability and excellent adhesion over a wide temperature range is developed. PA, as a proton donor center, endows the hydrogels with high conductivity (102.0 mS cm-1) based on the Grotthuss mechanism. PA can also prevent the crystallization of water and form multiple reversible hydrogen bonds in the polymer network, which solves the dysfunction of self-healing hydrogels in a cryogenic environment. Accordingly, the hydrogel electrolytes demonstrate fast low-temperature self-healing ability with a self-healing efficiency of 79.4% within 3 h at -20 °C. In addition, the hydrogel electrolytes present outstanding adhesiveness on electrodes due to the generation of hydrogen bonds between PA and activated carbon electrodes. As a result, the integrated hydrogel-based supercapacitors with tight bonding electrode/electrolyte interface deliver a 139.5 mF cm-2 specific capacitance at 25 °C. Moreover, the supercapacitors display superb self-healing ability, achieving 92.1% of capacitance recovery after three cutting-healing cycles at -20 °C. Furthermore, the supercapacitors demonstrate only 6.4% capacitance degradation after 5000 charging-discharging cycles at -20 °C. This work provides a roadmap for designing all-in-one flexible energy storage devices with excellent self-healing ability over a wide temperature range.

An adaptive waterborne fluorocarbon coatings with Anti-Flashing Rust, Antibiofouling, and Self-Repairing properties

Waterborne fluorocarbon coatings are gaining popularity as a more environmentally friendly replacement for traditional solvent-based coatings because of its corrosion resistance and antibiofouling properties. However, the environmental unfriendliness of small molecular emulsifiers used, the occurrence of flash rusting, and the inability to self-repair after accidental damage restrict its application in the marine industry. Here, a redox-responsive copolymer (PMx) was synthesized by the amphiphilic nature of waterborne polyurethane as microreactors, which was employed as coatings (PMx/WPU) with anti-flashing rust, antibiofouling, and self-repairing functions. The copolymer was polymerized from chlorotrifluoroethylene (CTFE), vinyl acetate (VA), and a special monomer conjugated to the corrosion inhibitor 2-benzothiazolethiol (MBT) through disulfide bonds, in which MBT can be released through disulfide bond breaking in a reducing environment, effectively preventing the occurrence of flash rusting. The combination of the repelling properties of the fluorinated groups and the bactericidal action of the MBT results in PMx/WPU coatings with excellent antibiofouling properties. Additionally, the reversible hydrogen bonds in the polyurethane provide the PMx/WPU coatings with excellent self-repairing ability (93.9%). Our study presents a new approach to polymerize fluoro-substituted ethylene monomers using polyurethane as microreactors, enabling the preparation of waterborne fluorocarbon coatings with anti-flashing rust, antibiofouling, and self-repairing properties for practical applications.

Developing multifunctional pectin-based hydrogel for wound dressing: In silico, in vitro and in vivo evaluation

Multifunctional hydrogel wound dressing with high hemostatic, antioxidant, and self-healing activity is desirable in clinical applications. In this contribution, we developed two distinct hydrogel formulations, namely PZ and PTBA, by employing low methoxyl pectin (P), zeolite, or 2-thiobarbituric acid (TBA) for sustained release of procaine (PC) in a controlled manner up to 40 h. These hydrogel systems (PZ and PTBA) utilize dynamic reversible hydrogen bonds between the components and a metal coordination bond between carboxyl acid groups of pectin chains and Ca2+ to confer self-healing properties, as demonstrated by molecular dynamics (MD) and rheological analyses. Moreover, PZ and PTBA hydrogels possess superior antioxidant, hemostasis, biocompatibility, and antibacterial activities. The data from the mouse skin incision model and infected full-thickness skin wound model demonstrated the highest wound closure rate (wound closure area per day) was achieved by the PZ (4.72) and PTBA (4.62) groups on day 21, which was better than the control (4.2) and Kaltostat groups (4.05) (p < 0.05). PZ and PTBA’s effectiveness in wound closure and acceleration of the wound healing process, highlighting its significant potential in wound management.

Moisture self-regulating ionic skins with ultra-long ambient stability for self-healing energy and sensing systems

Dehydration has been a key limiting factor for the operation of conductive hydrogels in practical application. Here, we report self-healable ionic skins that can self-regulate their internal moisture level by capturing extenral moistures via hygroscopic ion-coordinated polymer backbones through antipolyelectrolyte effect. Results show the ionic skin can maintain its mechanical and electrical functions over 16 months in the ambient environment with high stretchability (fracture stretch ∼2216 %) and conductivity (23.5 mS/cm). The moisture self-regulating capability is further demonstrated by repeated exposures to harsh environments such as 200°C heating, freezing, and vacuum drying with recovered conductivity and stretchability. Their reversible ionic and hydrogen bonds also enable self-healing feature as a sample with the fully cut-through damage can restore its conductivity after 24 h at 40 % relative humidity. Utilizing the ionic skin as a building block, self-healing flexible piezoelecret sensors have been constructed to monitor physiological signals. Together with a facile transfer-printing process, a self-powered sensing system with a self-healable supercapacitor and humidity sensor has been successfully demonstrated. These results illustrate broad-ranging possibilities for the ionic skins in applications such as energy storage, wearable sensors, and human-machine interfaces.

Liquid metal-enhanced self-healing dual-hard-phase cross-linked waterborne polyurethane for flexible sensors

Flexible strain sensors are increasingly recognized in areas such as health monitoring, mechanical operations, and infrastructure due to their ability to detect minute mechanical signals and conform to irregular surfaces. As sophisticated smart materials, these sensors demand exceptional sensitivity, durability, and robust self-healing capabilities. In this paper, methyl 2,6-dihydroxybenzoate and 2,2′-diaminodiphenyl disulfide were introduced into waterborne polyurethane to form a dual-hard-phase crosslinked matrix, which is characterized by dynamic covalent disulfide bonds and reversible hydrogen bonds. The resultant WPU-D5B2 material exhibits outstanding tensile strength (34.80 MPa) and toughness (190.5 MJ m−3), with a 97.4 % degree of self-healing at 50 ℃ for 2 h. Remarkably, this material maintains 83 % of its original mechanical performance even following recycling processe. This method significantly enhances the performance of flexible strain sensors in complex environments. Consequently, a composite conductor was prepared by blending self-healing waterborne polyurethane (WPU), graphene oxide (GO), and liquid metal (LM). Graphene oxide formed an efficient electronic conductive network, while liquid metal served as a conductive medium, filling microgaps to maintain the integrity of the electron pathway. This innovative dual-conductive mechanism ensures reliable performance in applications such as advanced flexible sensors.

Multistimuli responsive hydrogels with shape fix/memory capability fabricated from gold nanorod‐conjugated amino acid‐based vinyl polymer networks

AbstractFabricating robust shape‐memory hydrogels that respond to multiple external stimuli is an important challenge in facilitating gel technology for versatile applications. In this study, we report a simple approach for constructing thermo‐, redox‐, and photo‐responsive hydrogels with high mechanical strength and shape fix/memory capability. Upper critical solution temperature (UCST)‐type amino acid‐based hydrogels were facilely prepared by radical copolymerization of N‐acryloyl glycinamide (NAGAm) with cystine‐derived divinyl acrylamides (ionic cystine [NAC] or nonionic cystine‐methyl ester [NACMe]) units at different monomer concentrations (1/2 M). These hydrogels were transparent and exhibited good mechanical strength (tensile strength of 0.3–0.4 MPa and breaking elongation of 400%–700%). All hydrogels showed UCST‐type swelling‐shrinking behaviors based on thermo‐driven reversible hydrogen bonds among the PNAGAm units, and thus could be fixed into variety of shapes and recovered to the original shape by temperature manipulation. The cystine‐based crosslinkers having SS bonds served as efficient redox‐sensitive and gold‐nanorod‐(AuNR)‐adsorbing moieties; thus, AuNR could be conjugated stably and evenly into the PNAGAm/NAC hydrogel. Moreover, upon light‐irradiation, the AuNR‐conjugated hybrid hydrogel exhibited shape‐memory behavior owing to the photothermal effect of the AuNRs. These multiresponsive/functional hydrogels composed of amino acid units have considerable potential for various applications in the fields of soft actuators and biomedicines.

A Self-Healing Polymer Binder of Silicon-Based Anode with Enhanced Lithium-Ion Transport Performance

A multi-functional binder was designed for silicon-based anode lithium-ion battery to alleviate the huge volume expansion of silicon anode during the process of charging and discharging, and to provide ion transport channels to improve the rate performance of electrodes to meet the needs of rapid charging and discharging. In this study, a binder PAA-TUEG which combined the mechanical properties of PAA, the fast self-healing ability provided by the zigzag hydrogen bond in TUEG, and the ion transport ability provided by the ether-oxygen group was synthesized. The effect of different proportion of TUEG binder on the electrochemical performance of the electrode was further investigated. The synthesized PAA-TUEG5% polymer material exhibits a tensilestrength of 0.8 MPa and a fracture elongation of 397%. The Si@PAA-TUEG5% electrode demonstrates reversible capacities of 3035, 2260, and 1249 mAh g−1 at 0.5, 1, and 2 C (1 C = 3500 mAh g−1), respectively. In extended cycling tests, the remaining capacities after 180 cycles at 0.5 and 1 C are 852 and 793 mAh g−1, respectively. This innovative binder, featuring both self-healing ability and enhanced ion transport through dynamic reversible hydrogen bond and ionic bond, presents a promising design concept for the next generation of high-energy-density lithium-ion batteries.

Structural Design and Energy and Environmental Applications of Hydrogen-Bonded Organic Frameworks: A Systematic Review.

Hydrogen-bonded organic frameworks (HOFs) are emerging porous materials that show high structural flexibility, mild synthetic conditions, good solution processability, easy healing and regeneration, and good recyclability. Although these properties give them many potential multifunctional applications, their frameworks are unstable due to the presence of only weak and reversible hydrogen bonds. In this work, the development history and synthesis methods of HOFs are reviewed, and categorize their structural design concepts and strategies to improve their stability. More importantly, due to the significant potential of the latest HOF-related research for addressing energy and environmental issues, this work discusses the latest advances in the methods of energy storage and conversion, energy substance generation and isolation, environmental detection and isolation, degradation and transformation, and biological applications. Furthermore, a discussion of the coupling orientation of HOF in the cross-cutting fields of energy and environment is presented for the first time. Finally, current challenges, opportunities, and strategies for the development of HOFs to advance their energy and environmental applications are discussed.

A Hydrogen-Bonded, Hexagonally Networked, Layered Framework with Large Aperture Designed by Structural Synchronization of a Macrocycle and Supramolecular Synthon.

To develop porous organic frameworks, precise control of the stacking manner of two-dimensional porous motifs and structural characterization of the resultant framework are important. From these points of view, porous molecular crystals formed through reversible intermolecular hydrogen bonds, such as hydrogen-bonded organic frameworks (HOFs), can provide deep insight because of their high crystallinity, affording single-crystalline X-ray diffraction analysis. In this study, we demonstrate that the stacking manner of hydrogen-bonded hexagonal network (HexNet) sheets can be controlled by synchronizing a homological triangular macrocyclic tecton and a hydrogen-bonded cyclic supramolecular synthon called the phenylene triangle. A structure of the resultant HOF was crystallographically characterized and revealed to have a large channel aperture of 2.4 nm. The HOF also shows thermal stability up to 290 °C, which is higher than that of the conventional HexNet frameworks.

A room‐temperature self‐healing anticorrosion coating of supramolecular polyurethane based on dynamic reversible quadruple hydrogen bond

AbstractThe contradiction between the migration rate of molecular chains and mechanical strength has always been a key factor affecting the practical application of self‐healing anticorrosion coatings. In this paper, a series of supramolecular self‐healing elastomers (SPU‐MP) were prepared by the reaction of diphenylmethane diisocyanate and polyether amine. The results shown that the proportion of polyetheramine D230 (D230) in molecular segments affects the hydrogen bond density between molecular chains, thereby affecting the self‐healing efficiency and mechanical strength of SPU‐MP. When the ratio of D230 and polyetheramine D400 (D400) is 2:8, the tensile fracture strength of SPU‐MP8 is 5.08 MPa, and the self‐healing efficiency reaches 82.1% after 10 h of repair at room temperature. Further increasing the ratio of D230 increases the relaxation time of the molecular chain due to the increase in hydrogen bond density, resulting in a decrease in the self‐healing efficiency of SPU‐MP. The results of electrochemical experiments and neutral salt spray experiments indicate that the anticorrosion coating prepared by SPU‐MP8 exhibits good self‐healing performance. After immersing in 3.5 wt.% NaCl solution for 35 days, the low‐frequency impedance modulus of the intact coating and the scratch coating were both higher than 107 Ω cm2, still shown good anticorrosion ability.

Biomimetic Design of Hydration‐Responsive Silk Fibers and their Role in Actuators and Self‐Modulated Textiles

AbstractHydration‐induced shape‐morphing behavior has been discovered in many natural fiber‐based materials, yet this smart behavior in regenerated fibers from biopolymers lacks investigation. Here, hierarchically structured silk fibers are developed with anisotropic long‐range molecular organization and water‐responsive effects resembling natural spider silk. The regenerated silk fibers exhibit the water‐triggered shape‐memory effect and a water‐driven cyclic response. The reversible hydrogen bonds and transformation in the metastable secondary structure from α‐helices/random coils to β‐sheets are explored as the mechanisms responsible for the water‐responsiveness. The silk fibers obtained possess a tensile strength higher than 104 MPa at a fracture strain of ≈100%, showing noticeable toughness. The water‐responsive silk fibers exhibit a shape recovery rate of ∼83% and generate a maximum actuation stress of up to 18 MPa during the water‐driven cyclic contraction that outperforms most traditional natural textile fibers. The regenerated silk fibers show potential for use in water‐driven actuators, artificial muscle, and smart fabrics based on the integration of suitable mechanical properties and water responsiveness.