Synthetic biology enables the precise design of protein-based materials with modular sequences and tailored functionality, offering new potential for surgical applications. Moreover, three-dimensional (3D) printing is emerging as a powerful platform for fabricating biomedical materials with tunable structure and composition. In this study, we evaluated a synthetic biology-engineered silk-amyloid-mussel foot (SAM) recombinant protein for fabrication of 3D printed hydrogel material, by glycidyl methacrylate (GMA) modification and UV crosslinking. Using extrusion-based 3D printing, hydrogels were fabricated and assessed for mechanical integrity, elasticity and adhesion. Hydrogels using silk fibroin (SF) with the same GMA crosslinking fabrication were used as control. SAM-based 3D printed hydrogels demonstrated superior modulus, elasticity, tissue adhesion, and energy dissipation, compared with SF. Overall, this comparative study explored the impact of protein molecular design and demonstrates the advantages of synthetic biology–derived proteins in engineering multifunctional, printable hydrogels for further biomedical applications.