Underwater adhesives receive extensive attention due to their wide applications in marine explorations and various related industries. However, current adhesives still suffer from excessive water absorption and lack of spontaneity. Herein, we report an autonomous underwater adhesive based on poly(2-hydroxyethyl methacrylate-co-benzyl methacrylate) amphiphilic polymeric matrix swollen by hydrophobic imidazolium ionic liquid. The as-prepared adhesive is tough and flexible, showing little to none instantaneous underwater adhesion onto the PET substrate, whereas its adhesion energy on the substrate can grow more than 5 times to 458 J·m⁻² after 24 hours. More importantly, this process is entirely spontaneous, without any external pressing force. Our comprehensive studies based on experimental characterizations and molecular dynamic simulations confirm that such autonomous adhesion process is driven by water-induced rearrangement of the functional groups. It is believed that such material can provide insights into the development of next-generation smart adhesives.

水下胶粘剂因其在海洋勘探及各相关行业的广泛应用而受到广泛关注。然而，目前的粘合剂仍然存在吸水率过高且缺乏自粘性的问题。在此，我们报道了一种基于聚（甲基丙烯酸2-羟乙酯-甲基丙烯酸苄酯）两亲性聚合物基质的自主水下粘合剂，该基质被疏水性咪唑鎓离子液体溶胀。所制备的粘合剂坚韧且柔韧，在 PET 基材上几乎没有瞬时水下粘合力，而其在基材上的粘合能在 24 小时后可增长 5 倍以上，达到 458 J·m ^-2。更重要的是，这个过程完全是自发的，没有任何外来的压力。我们基于实验表征和分子动力学模拟的综合研究证实，这种自主粘附过程是由水诱导的官能团重排驱动的。相信这种材料可以为下一代智能粘合剂的开发提供见解。