Strong, healable materials with bio‐like ordered architectures and versatile functionality

Abstract The capacity of biological tissues to undergo self‐healing is crucial for the performance of functions and the continuation of life. Conventional intrinsic self‐healing materials demonstrate analogous functionality depending on the dissociation‐recombination of reversible bonds with no need of extra repair agents. However, the trade‐off relationship between mechanical strength and self‐healing kinetics in intrinsic self‐healing systems, coupled with the lack of additional functionality, restricts their service life and practical applications. Diversified highly ordered structures in organisms significantly affect the energy dissipation mechanism, signal transmission efficiency, and molecular network reconstruction capability due to their multi‐dimensional differentiated macroscopic composite constructions, microscopic orientation textures, and topologies/bonding types at molecular level. These architectures exhibit distinctive strengthening mechanisms and functionalities, which provide valuable references. This review aims at providing the current status of advanced intrinsic self‐healing materials with biomimetic highly ordered internal micro/nanostructures. Through highlighting specific examples, the classifications, design inspirations, and fabrication strategies of these newly developed materials based on integrating dynamic interactions with ordered nano/microstructures are outlined. Furthermore, the strengthening and self‐healing balance mechanisms, structure–functionalization relationships, and potential application values are discussed. The review concludes with a perspective on the challenges, opportunities, and prospects for the development, application, and promotion of self‐healable materials with bio‐like ordered architectures.