In the present study, a polysaccharide metallohydrogel was successfully fabricated using succinoglycan and trivalent chromium and was verified via Fourier transform infrared spectroscopy, differential scanning calorimetry analysis, thermogravimetric analysis (TGA), field emission scanning electron microscopy, and rheological measurements. Thermal behavior analysis via TGA indicated that the final mass loss of pure succinoglycan was 87.8% although it was reduced to 65.8% by forming a hydrogel with trivalent chromium cations. Moreover, succinoglycan-based metallohydrogels exhibited improved mechanical properties based on the added concentration of Cr3+ and displayed a 10 times higher compressive stress and enhanced storage modulus (G′) of 230% at the same strain. In addition, the pore size of the obtained SCx could be adjusted by changing the concentration of Cr3+. Gelation can also be adjusted based on the initial pH of the metallohydrogel formulation. This was attributed to crosslinking between chromium trivalent ions and hydroxyl/carboxyl groups of succinoglycan, each of which exhibits a specific pH-dependent behavior in aqueous solutions. It could be used as a soft sensor to detect Cr3+ in certain biological systems, or as a soft matrix for bioseparation that allows control of pore size and mechanical strength by tuning the Cr3+ concentration.