Core–Shell Nanostructured Assemblies Enable Ultrarobust, Notch‐Resistant and Self‐Healing Materials

Abstract Actuators based on stimulus‐responsive soft materials have attracted widespread attention due to their significant advantages in flexibility and structural adaptability over traditional rigid actuators. However, the development of fast‐actuating, mechanical robust and self‐healing actuators without compromising flexibility remains an ongoing challenge. Here, this study presents a photo‐responsive flexible actuator by incorporating core–shell liquid metal nano‐assemblies into a polyurethane matrix to construct a dynamic supramolecular interface. The nano‐assemblies are endowed with adaptive characteristics to external loading, being expected to dissipate energy via the reversible reconstruction of hydrogen bonding and deformation of nano‐assemblies. The obtained composites exhibit excellent mechanical strength (31 MPa), low modulus (2.02 MPa), high stretchability (1563.95%), autonomous self‐healing (92.5%), and NIR‐responsive actuation properties. Furthermore, the combination of high cohesive energy but fluxible nano‐liquid metal core, and strong dynamic interface not only achieves the balance of high tensile strength and high flexibility but also endows the actuators with outstanding notch‐resistant performance (fracture energy≈58.8 kJ m −2 ) through multiphase energy dissipation. This work provides a promising strategy for developing soft yet tough self‐healing materials in the fields of flexible robotics and artificial muscles.