The introduction of glass matrix ceramics in dental restorations has revolutionized dental aesthetics. A key challenge in the development of dental glass ceramics is achieving nanocrystalline glass ceramics with superior mechanical properties without compromising translucency. In this study, ZrO2-SiO2 glass ceramics doped with amorphous Al2O3 were investigated to address these requirements. The results indicate that the segregation of Al3+ at the grain boundaries of ZrO2 crystallites and the nano-domains of amorphous Al2O3 significantly influences the microstructure, including the grain size and stabilization of tetragonal ZrO2, as well as the translucency and mechanical properties. The composition with 10 mol% Al2O3 exhibits the highest toughness of 8.05 MPa center dot m1/2 while maintaining excellent translucency. Moreover, the composition with 5 mol% Al2O3 demonstrates lower translucency but achieves a high flexural strength of 960 MPa. Overall, the mechanical properties of these translucent glass matrix ceramics surpass those of commercially available dental glass ceramics, highlighting their potential for dental restoration applications.