Bioinspired Mechanically Robust and Recyclable Hydrogel Microfibers Based on Hydrogen‐Bond Nanoclusters

Abstract Mechanically robust hydrogel fibers have demonstrated great potential in energy dissipation and shock‐absorbing applications. However, developing such materials that are recyclable, energy‐efficient, and environmentally friendly remains an enormous challenge. Herein, inspired by spider silk, a continuous and scalable method is introduced for spinning a polyacrylamide hydrogel microfiber with a hierarchical sheath‐core structure under ambient conditions. Applying pre‐stretch and twist in the as‐spun hydrogel microfibers results in a tensile strength of 525 MPa, a toughness of 385 MJ m −3 , and a damping capacity of 99%, which is attributed to the reinforcement of hydrogen‐bond nanoclusters within the microfiber matrix. Moreover, it maintains both structural and mechanical stability for several days, and can be directly dissolved in water, providing a sustainable spinning dope for re‐spinning into new microfibers. This work provides a new strategy for the spinning of robust and recyclable hydrogel‐based fibrous materials.