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Fabrication of anisotropic hydrogels exhibiting direction-dependent structure and properties has attracted great interest in biomimicking, tissue engineering, and bioseparation. Herein, we report a freeze-casting-based fabrication of structurally and mechanically anisotropic aerogels and hydrogels composed of hydrazone cross-linked poly(oligoethylene glycol methacrylate) (POEGMA) and cellulose nanocrystals (CNCs). We show that, by controlling the composition of the CNC/POEGMA dispersion and the freeze-casting temperature, aerogels with fibrillar, columnar, or lamellar morphologies can be produced. Small-angle X-ray scattering experiments show that the anisotropy of the structure originates from the alignment of the mesostructures, rather than the CNC building blocks. The composite hydrogels show high structural and mechanical integrity and a strong variation in Young’s moduli in orthogonal directions …