High strength, high stiffness and toughness, defect‐tolerant waterborne polyurethane with healing and antibacterial abilities

Abstract The nature creates many biomaterials such as spider silk which exhibits a combination of stiffness, strength and toughness. However, most of synthetic unfilled materials suffer from a trade‐off between toughness and stiffness. Inspired by the structure of spider silk but beyond it, we proposed a novel molecular design to achieve transparent unfilled waterborne polyurethane (WPU) with simultaneously enhanced stiffness (280.9 MPa), tensile strength (25.1 MPa) and toughness (140.0 MJ/m 3 ) as well as good elasticity (710%). The designed WPU comprised homogeneous continuous phase (soft segments) and diverse H‐bonds (hard segments) dispersed in it. The increase of rigid molecular chain content and H‐bonds contributed to the high stiffness of WPU. Furthermore, the mismatch of stiffness between hard domains and soft segments might promote crack deflection and branching, which endowed the robust WPU with fracture energy of 81.16 kJ/m 2 . The robust WPU film could be healed to recover most of its original mechanical properties (strength for 24.4 MPa and elongation for 610%) under heating. In addition, the WPU films demonstrated good antibacterial performance against Staphylococcus aureus and Escherichia coli after chlorination.