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.

Self‐Healing Elastomers Soft electronics seek all‐around high mechanical performance universal self‐healing elastomers. In article number 2103235, Jarkko Tolvanen and co‐workers report design strategy to achieve tough and resilient universal self‐healing elastomer. The resilin‐inspired bimodal siloxane‐based elastomer benefits from combination of soft and hard phases. The cover displays existing phase‐separated morphology during shape recovery captured by optical microscopy.

Organic Conductors Achieving excellent electrical, mechanical, and self‐healing properties with soft conductor has been challenging so far. In article number 2205485 , Jarkko Tolvanen and co‐workers report a co‐continuous multiphase design strategy for self‐healable organic conductor‐elastomer blend that achieves a good overall performance. The cover displays structure of the heterogenous multiphase conductor with microdroplet morphology captured by optical microscopy.

Next-generation, truly soft, and stretchable electronic circuits with material level self-healing functionality require high-performance solution-processable organic conductors capable of autonomously self-healing without external intervention. A persistent challenge is to achieve required performance level as electrical, mechanical, and self-healing properties optimized in tandem are difficult to attain. Here heterogenous multiphase conductor with cocontinuous morphology and macroscale phase separation for ultrafast universally autonomous self-healing with full recovery of pristine tensile and electrical properties in less than 120 and 900 s, respectively, is reported. The multiphase conductor is insensitive to flaws under stretching and achieves a synergistic combination of conductivity up to ≈1.5 S cm −1 , stress at break ≈4 MPa, toughness up to >81 MJ m −3 , and elastic recovery exceeding 2000% strain. Such properties are difficult to achieve simultaneously with any other type of material so far. The solution-processable multiphase conductor offers a paradigm shift for damage tolerant and environmentally resistant soft electronic components and circuits with material level self-healing.

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