Gelatin methacryloyl (GelMA) hydrogels are widely recognized for their biocompatibility, biodegradability, and tunable properties, making them promising candidates for biomedical applications, including bone tissue engineering, ocular therapies, endodontic treatment and drug delivery. However, their inherent mechanical fragility and rapid degradation limit their use in load-bearing or long-term biological environments. This research addresses these limitations by incorporating fumed silica nanoparticles into GelMA hydrogels to enhance mechanical stiffness, and, by leveraging Volumetric Additive Manufacturing (VAM) for support-free 3D fabrication of geometrically complex constructs such as gyroid unit cells. This study formulated silica-toughened index-matched GelMA hydrogels with higher sheer storage modulus, increased compressive stiffness, and prolonged swelling stability, hence allowing improved mechanical properties, improved rheological behavior and controlled degradation while preserving the hydrogel’s printability via UV-based photopolymerization. These hydrogels were successfully printed using a tomographic VAM technique called Computed Axial Lithography (CAL), which enables high-resolution structures without the constraints of traditional layer-by-layer methods. This thesis offers a dual innovation: the creation of a mechanically robust, biofunctional hydrogel and the demonstration of its compatibility with VAM-based printing. The integration of silica nanoparticle reinforcement with volumetric fabrication represents a step forward in the manufacturing of next-generation biomedical devices and regenerative therapies.