Poly(methyl methacrylate) (PMMA) is widely used in dental applications. However, PMMA specialized for stereolithography (SLA) additive manufacturing (3D-printing) has not been developed yet. This study aims to develop a novel PMMA-based resin for SLA 3D-printing by mixing methyl methacrylate (MMA), ethylene glycol dimethacrylate (EGDMA), and PMMA powder in various mixing ratios. The printability and the viscosity of the PMMA-based resins were examined to determine their suitability for 3D-printing. The mechanical properties (flexural strength and Vickers hardness), shear bond strength, degree of conversion, physicochemical properties (water sorption and solubility), and cytotoxicity for L929 cells of the resulting resins were compared with those of three commercial resins: one self-cured resin and two 3D-print resins. EGDMA and PMMA were found to be essential components for SLA 3D-printing. The viscosity increased with PMMA content, while the mechanical properties improved as EGDMA content increased. The shear bond strength tended to decrease as EGDMA increased. Based on these characteristics, the optimal composition was determined to be 30% PMMA, 56% EGDMA, 14% MMA with flexural strength (84.6 ± 7.1 MPa), Vickers hardness (21.6 ± 1.9), and shear bond strength (10.5 ± 1.8 MPa) which were comparable to or higher than those of commercial resins. The resin’s degree of conversion (71.5 ± 0.7%), water sorption (19.7 ± 0.6 μg/mm3), solubility (below detection limit), and cell viability (80.7 ± 6.2% at day 10) were all acceptable for use in an oral environment. The printable PMMA-based resin is a potential candidate material for dental applications.