Bioinspired Hierarchical Hydrogels Engineered with Extreme Impact Resistance

Abstract The development of extreme impact‐resistant materials holds significant importance across engineering applications, yet remains constrained by the inherent trade‐offs among mechanical strength, toughness, and energy dissipation efficiency. Drawing inspiration from natural models, particularly the unique structural design and toughening mechanisms of the mantis shrimp's dactyl club, a kind of nanocomposite hydrogel is developed by synergistically integrating polymer elastic microspheres with enzyme‐induced biomineralization. This bioinspired approach produces microsphere‐reinforced nanocomposite hydrogels (MNHs) that concurrently deliver exceptional strength, remarkable fracture toughness, and unprecedented resistance to ballistic impacts, surpassing the performance of all existing high‐strength hydrogels, thus underscoring their potential for protective applications. Nonlinear numerical and theoretical analyses elucidate the dynamic fracture mechanisms governing both quasi‐static and high‐speed impact scenarios, revealing crack deflection, microcrack nucleation, and energy redistribution as key toughening pathways. This work not only advances the fundamental understanding of bioinspired structural design principles but also establishes a universal blueprint for next‐generation impact‐resistant materials, unlocking new frontiers for polymer composites in mechanically demanding scenarios.