Room‐Temperature Self‐Healing Soft Composite Network with Unprecedented Crack Propagation Resistance Enabled by a Supramolecular Assembled Lamellar Structure

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.