Abstract Despite their potential in ionic electronics, conventional ionic conductors face critical limitations, including modest strain‐modulated conductivity and restricted self‐regulation under temperature variations. Here, a mechanically robust all‐solid‐state ionic elastomer is presented, engineered through molecular design and microphase separation. By in situ integrating polyacrylamide (PAM) and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) into maleic anhydride‐grafted styrene‐ethylene‐butylene‐styrene (SEBS‐MAH), a hierarchical structure with dynamic non‐covalent interactions (hydrogen bonds, lithium bonds, and cation‐π effects) is achieved. This design yields exceptional mechanical properties, including a tensile strength of 46.4 MPa, strain of 1066%, and toughness of 207.8 MJ m −3 , alongside outstanding recyclability and puncture resistance. Remarkably, strain‐induced alignment of microphase‐separated domains reduces ion transport tortuosity, enabling a 1300 times conductivity enhancement at 1066% strain. Concurrently, temperature‐gated ion release from confined regions triggers a 1600 times conductivity increase at 120 °C. The elastomer maintains high conductivity (>10 −3 S m −1 ) across an ultra‐wide temperature range (−45–120 °C), overcoming the limitations of conventional hydrogels and ionogels. This work pioneers a dual‐stimuli‐responsive strategy for advanced ionic conductors, offering transformative potential in wearable electronics, soft robotics, and adaptive sensors.
Yang et al. (2025) studied this question.