Stretch‐Induced Conductivity Enhancement in Highly Conductive and Tough Hydrogels

Abstract The resistance of gels and elastomers increases significantly with tensile strain, which reduces conductive stability and restricts their use in stable and reliable electronics. Here, highly conductive tough hydrogels composed of silver nanowires (AgNWs), liquid metal (LM), and poly(vinyl alcohol) (PVA) are fabricated. The stretch‐induced orientations of AgNWs, deformable LM, and PVA nanocrystalline create conductive pathways, enhancing the mechanical properties of the hydrogels, including increased ultimate fracture stress (13‐33 MPa), strain (3000–5300%), and toughness (390.9–765.1 MJ m −3 ). Notably, the electrical conductivity of the hydrogels is significantly improved from 4.05 × 10 −3 to 24 S m −1 when stretched to 4200% strain, representing a 6000‐fold enhancement. The incorporation of PVA nanocrystalline, deformable LM, and AgNWs effectively mitigates stress concentration at the crack tip, thereby conferring crack propagation insensitivity and fatigue resistance to the hydrogels. Moreover, the hydrogels are designed with a reversible crosslinking network, allowing for water‐induced recycling.