- Cryotropic gelation is one of the most common approaches to design novel hydrogels with multifaceted technological and biological functionalities. In the present paper, we studied the ability of highly galactosyl-substituted galactomannans, i.e. fenugreek and alfalfa gum, to form physically crosslinked hydrogels via cryogenic processing. Cycling of the galactomannan solutions (0.25 to 4% wt) from 25 to −20 to 25 °C induced the physical crosslinking of the galactomannan chains leading to the formation of different cryogel structures, i.e. filamentous aggregates (c* < c < 1%), cellular-like gel networks (1 ≤ c < 4%) or a homogeneously swollen gel (c ≥ 4%), depending on the total biopolymer content. Alfalfa gum-based cryogels exhibited higher elasticity and stiffness, better uniformity of the structure and a lower macropore size than their fenugreek counterparts. The physical blending of alfalfa or fenugreek gum with locust bean gum (2% total biopolymer) led to the reinforcement of the mechanical properties of the cryogels without significantly altering their microstructural aspects.