3D printing techniques are increasingly being explored to produce hydrogels, versatile materials with a wide range of applications. While photopolymerization-based 3D printing can produce customized hydrogel shapes and intricate structures, its reliance on rigid printing conditions limits material properties compared to those of extrusion printing. To address this limitation, this study employed an alternative approach by printing an organogel precursor using vat polymerization with organic solvents instead of water, followed by solvent exchange after printing to create the final hydrogel material. Using mask stereolithography (mSLA), we evaluated the effects of solvent choice on a novel and recently developed 3D-printed supramolecular hydrogel, cross-linked with quaternized chitosan/acrylate salt. In this study, we compared the conventional solvent dimethyl sulfoxide (DMSO) with the bioderived solvent Cyrene. Our findings reveal that hydrogels produced with Cyrene-based 3D printing exhibit weaker strength but high swelling capacity and elasticity, resilience to cyclic loading, and the ability to produce detailed and accurate 3D-printed objects. These results provide insights into the solvent-dependent mechanical and physical characteristics of 3D-printed hydrogels and underscore the potential of Cyrene as a sustainable alternative for polymeric synthesis.