Impact‐Resistant Hydrogels by Harnessing 2D Hierarchical Structures

With the strengthening capacity through harnessing multi-length-scale structural hierarchy, synthetic hydrogels hold tremendous promise as a low-cost and abundant material for applications demanding unprecedented mechanical robustness. However, integrating high impact resistance and high water content, yet superior softness, in a single hydrogel material still remains a grand challenge. Here, a simple, yet effective, strategy involving bidirectional freeze-casting and compression-annealing is reported, leading to a hierarchically structured hydrogel material. Rational engineering of the distinct 2D lamellar structures, well-defined nanocrystalline domains and robust interfacial interaction among the lamellae, synergistically contributes to a record-high ballistic energy absorption capability (i.e., 2.1 kJ m ), without sacrificing their high water content (i.e., 85 wt%) and superior softness. Together with its low-cost and extraordinary energy dissipation capacity, the hydrogel materials present a durable alternative to conventional hydrogel materials for armor-like protection circumstances.