Bilayer zirconia restoration is one of the most commonly used restorations in dental practice, but the high frequency of the cohesive/adhesive fracture of veneered porcelain is still a problem. This paper focuses on the development of nanostructured glass-zirconia to improve the interface stability of dental zirconia substrate and veneered porcelain. A novel SiO₂-Li₂O-Al₂O₃ (SLA) glass was prepared and infiltrated into the surface of fully sintered dental zirconia to obtain nanostructured glass-zirconia structure. The prepared glass-zirconia was analyzed with scanning electron microscopes (SEM), energy dispersive spectroscopy (EDS) and X-ray diffraction spectroscopy (XRD). The wettability, roughness and 3D morphology of zirconia were altered, and shear bonding strength (SBS) test demonstrated almost double increase in SBS values of the nanostructured glass-zirconia structure. The failure modes and microstructure characteristics also verified the improved interfacial stability. This investigation provides a promising method for enhancing the structural stability of bilayer zirconia restorations.