Soft self-healing materials are compelling candidates for stretchable devices because of their excellent compliance, extensibility, and self-restorability. However, most existing soft self-healing polymers suffer from crack propagation and irreversible fatigue failure due to easy breakage of their dynamic amorphous, low-energy polymer networks. Herein, inspired by distinct structure-property relationship of biological tissues, a supramolecular interfacial assembly strategy of preparing soft self-healing composites with unprecedented crack propagation resistance is proposed by structurally engineering preferentially aligned lamellar structures within a dynamic and superstretchable poly(urea-ureathane) matrix (which is elongated to 24 750× its original length). Such a design affords a world-record fracture energy (501.6 kJ m −2 ), ultrahigh fatigue threshold (4064.1 J m −2 ), and outstanding elastic restorability (dimensional recovery from 13 times elongation), and preserving low modulus (1.2 MPa), high stretchability (3200%), and high room-temperature self-healing efficiency (97%). Thereby, the resultant composite represents the best of its kind and even surpasses most biological tissues. The lamellar 2D transition-metal carbide/carbonitride (MXene) structure also leads to a relatively high in-plane thermal conductivity, enabling composites as stretchable thermoconductive skins applied in joints of robotics to thermal dissipation. The present work illustrates a viable approach how autonomous self-healing, crack tolerance, and fatigue resistance can be merged in future material design.

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Adhesive hydrogels containing quaternary ammonium salt (QAS) moieties have shown attractive advantages in treatment for acute wounds, attributed to their high performances in wound sealing and sterilization. However, the introduction of QAS commonly leads to high cytotoxicity and adhesive deterioration. Herein, aimed to solve these two issues, a self‐adaptive dressing with delicate spatiotemporal responsiveness is developed by employing cellulose sulfate (CS) as dynamic layers to coat QAS‐based hydrogel. In detail, due to the acid environment of wound in the early stages of healing, the CS coating will quickly detach to expose the active QAS groups for maximum disinfectant efficacy; meanwhile, as the wound gradually heals and recovers to a neutral pH, the CS will remain stable to keep QAS screened, realizing a high cell growth‐promoting activity for epithelium regeneration. Additionally, attributed to the synergy of temporary hydrophobicity by CS and slow water absorption kinetics of the hydrogel, the resultant dressing possesses outstanding wound sealing and hemostasis performance. At last, this work anticipates this approach to intelligent wound dressings based on dynamic and responsive intermolecular interaction can also be applied to a wide range of self‐adaptive biomedical materials employing different chemistries for applications in medical therapy and health monitoring.