Multifunctional Polyurethane Exhibiting High Mechanical Performance and Shape‐Memory‐Assisted Self‐Healing

Abstract Polymeric materials often face inherent trade‐offs between mechanical performance and self‐healing capabilities, which presents significant challenges to their development and practical application. Here, an effective strategy is reported to overcome these limitations. By introducing a highly crystalline polyol—characterized by its chain folding and storage chain length—and coordination bonds into polyurethane, an exceptional balance of high tensile strength (47.18 ± 2.35 MPa), exceptional elongation at break (5952.72 ± 254.20%), outstanding toughness (1396.39 ± 90.05 MJ m −3 ), and high hardness (shore D hardness 43.8 ± 0.8) is achieved, while also maintaining intrinsic self‐healing properties. The material's self‐healing is facilitated by the water solubility of polyol (polyethylene glycol, PEG), which enables rapid healing and welding at low temperatures (4 °C) with the aid of water. Additionally, the shape‐memory recovery force further enhances crack closure and healing, contributing to the material's durability. This unique combination of mechanical performance and self‐healing capabilities underscores the potential of this material for advanced applications that require both high mechanical properties and robust self‐healing functionality.