Ultra‐Highly Stiff and Tough Shape Memory Polyurea with Unprecedented Energy Density by Precise Slight Cross‐Linking

Abstract Shape memory polymers (SMPs) have attracted significant attention and hold vast potential for diverse applications. Nevertheless, conventional SMPs suffer from notable shortcomings in terms of mechanical properties, environmental stability, and energy density, significantly constraining their practical utility. Here, inspired by the structure of muscle fibers, an innovative approach that involves the precise incorporation of subtle, permanent cross‐linking within a hierarchical hydrogen bonding supramolecular network is reported. This novel strategy has culminated in the development of covalent and supramolecular shape memory polyurea, which exhibits exceptional mechanical properties, including high…

• NN
  National Natural Science Foundation of China

  Awards: 52072177, 2022YFB3808800, 52272084, No. 52272084
• NK
  National Key Research and Development Program of China

  Award: 2022YFB3808800
• FR
  Fundamental Research Funds for the Central Universities

  Award: 2023102003