Defect Engineering‐Induced Creep‐Free Hyperelastic Gels

ABSTRACT Viscoelastic creep in elastomer originates fundamentally from the molecular‐scale slippage and disentanglement of polymer chains governed by weak intermolecular interactions and imperfect crosslinking. Consequently, residual strain generated by long‐term mechanical loading severely limits the mechanical stability of gel materials. In this study, we proposed a sub‐unit‐cell‐scale defect engineering induced toughening strategy for fabricating creep‐free hyperelastic hydrogels. Within the nanospaces created by linker and cluster defects in metal–organic frameworks (MOFs), strong confined interaction between in situ polymerized polymers and MOF crystals enables rapid self‐reinforcement and remarkable creep resistance. The as‐prepared hydrogels exhibited low hysteresis with full recovery under 99% compressive strain, negligible creep, and outstanding fatigue resistance over 25 000 loading cycles. These features render our hydrogels a promising candidate for drift‐free iontronic sensors, allowing long‐term stable monitoring in air, underwater, and other complex environments.