Ultra‐Tough Self‐Healing Hydrogel via Hierarchical Energy Associative Dissipation

Owing to high water content and homogeneous texture, conventional hydrogels hardly reach satisfactory mechanical performance. Tensile‐resistant groups and structural heterogeneity are employed to fabricate tough hydrogels. However, those techniques significantly increase the complexity and cost of material synthesis, and have only limited applicability. Here, it is shown that ultra‐tough hydrogels can be obtained via a unique hierarchical architecture composed of chemically coupled self‐assembly units. The associative energy dissipation among them may be rationally engineered to yield libraries of tough gels with self‐healing capability. Tunable tensile strength, fracture strain, and toughness of up to 19.6 MPa, 20 000%, and 135.7 MJ cm⁻(3) are achieved, all of which exceed the best known records. The results demonstrate a universal strategy to prepare desired ultra‐tough hydrogels in predictable and controllable manners.