Hydrogels consisting lots of water resemble the human soft tissues, but their disordered structures and weak mechanical properties usually limit their biomedical applications. Herein, a facile strategy to prepare highly ordered nanocomposite hydrogels with ultrahigh strength is reported, where the oriented tunicate cellulose nanocrystals (TCNCs) were locked in polymeric networks. Firstly, a stretchable supramolecular hydrogel was prepared by loosely crosslinking adamantine moiety contained polymers with β-cyclodextrin modified TCNCs through host-guest interaction. Subsequently, dual physically cross-linked hydrogel was constructed by introducing Fe³⁺ ions into the pre-stretched supramolecular hydrogel for the formation of coordination bonds and freezing of oriented TCNCs. The resultant hydrogels exhibited ultrahigh tensile strength, elastic modulus, and toughness, along the direction of pre-stretching. The aligned TCNCs as both multifunctional cross-linking agents and interfacial compatible reinforcements of dual physically cross-linked networks largely contributed to the excellent mechanical performance of nanocomposite hydrogel. Our findings provide a universal method for designing hydrogels with highly ordered architectures and outstanding mechanical performances as potential biomimetic materials for biomedical applications.

包含大量水的水凝胶类似于人体的软组织，但其无序的结构和较弱的机械性能通常会限制其生物医学应用。在本文中，报道了一种制备具有超高强度的高度有序的纳米复合水凝胶的简便策略，其中将定向的束缚纤维素纳米晶体（TCNC）锁定在聚合物网络中。首先，通过主体-客体相互作用，通过将含金刚烷部分的聚合物与β-环糊精修饰的TCNCs进行松散交联，制备了可拉伸的超分子水凝胶。随后，通过引入Fe ^3+来构建双重物理交联的水凝胶离子进入预拉伸的超分子水凝胶，以形成配位键并冻结定向的TCNC。所得的水凝胶沿预拉伸方向显示出超高的拉伸强度，弹性模量和韧性。作为多功能交联剂和双重物理交联网络的界面相容性增强物的对齐TCNC在很大程度上促进了纳米复合水凝胶的优异机械性能。我们的发现为设计具有高度有序结构和出色机械性能的水凝胶提供了一种通用方法，可作为生物医学应用中潜在的仿生材料。