23 MPa), despite its exceptionally high water content (i.e., 90 wt%). The integration of such unprecedented mechanical attributes is mainly ascribed to the exquisite multilayered lamellar structures consisting of aligned chitin nanofibers. [5,6] However, when compared with natural materials, conventional synthetic hydrogels are typically weak and fragile for practical applications, owing to the sparsely crosslinked network, low solid content, homogeneous structure, and absence of structural hierarchy, thus hampering their practical applications where long service life, high loading capability and/or impact tolerance are highly demanded. [7][8][9][10] One of the most promising approaches to engineer synthetic hydrogels with extraordinary mechanical properties (i.e., strength, modulus, toughness and fatigue resistance) is through the bioinspired structural hierarchy design. [10][11][12][13][14][15][16][17] The most spectacular examples are nacre-like polymer or hydrogel composites, which are consisted of aligned micro/nanoparticles in a polymer matrix, thus, enabling them stiff yet tough and able to dissipate energy. [5,[18][19][20][21][22][23] In addition to the layered and brick-and-mortar microstructures, high inorganic loading (i.e., >70 wt%) is another critical role for the mechanical enhancement, however, sacrificing 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 −1 ), 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.