All‐Around Universal and Photoelastic Self‐Healing Elastomer with High Toughness and Resilience

Ultimately soft electronics seek affordable and high mechanical performance universal self‐healing materials that can autonomously heal in harsh environments within short times scales. As of now, such features are not found in a single material. Herein, interpenetrated elastomer network with bimodal chain length distribution showing rapid autonomous healing in universal conditions (<7200 s) with high efficiency (up to 97.6 ± 4.8%) is reported. The bimodal elastomer displays strain‐induced photoelastic effect and reinforcement which is responsible for its remarkable mechanical robustness (≈5.5 MPa stress at break and toughness ≈30 MJ m(−3)). The entropy‐driven elasticity allows an unprecedented shape recovery efficiency (100%) even after fracturing and 100% resiliency up to its stretching limit (≈2000% strain). The elastomers can be mechanically conditioned leading to a state where they recover their shape extremely quickly after removal of stress (nearly order of magnitude faster than pristine elastomers). As a proof of concept, universal self‐healing mechanochromic strain sensor is developed capable of operating in various environmental conditions and of changing its photonic band gap under mechanical stress.