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Polymer-infiltrated ceramic network (PICN) materials have gained considerable attention as tooth restorative materials owing to their mechanical compatibility with human teeth. However, the mechanical strength of contemporary PICN materials is lower than those of conventional resin composites and ceramics. This study aims to develop novel high-strength PICN for use as a dental restorative material. Zirconia-based PICN (EXP) was fabricated using 3 mol% yttria tetragonal polycrystalline zirconia powder and resin monomers via slip casting, followed by sintering and polymer infiltration. Comprehensive analyses of the microstructure, mechanical properties, and physicochemical properties of EXP were performed using scanning electron microscopy with energy-dispersive X-ray spectroscopy, Fourier transform infrared spectroscopy, inorganic content measurements, three-point bending test, Vickers hardness test, two-body wear test, shear bond strength (SBS) test, surface free energy analysis, and water sorption/solubility test. Commercially available computer-aided design/computer-aided manufacturing (CAD/CAM) materials, including resin composite (CERASMART), silicate-based PICN (ENAMIC), and zirconia ceramic (e.max ZirCAD), were used for comparison. The analyses highlight the dual network structure of EXP, which comprised a zirconia skeleton and an infiltrated resin phase. EXP exhibits a flexural strength of 346.0 ± 46.0 MPa, flexural modulus of 44.0 ± 3.7 GPa, and Vickers hardness of 440.1 ± 51.2 VHN. The mechanical properties of EXP are significantly higher than those of CERASMART and ENAMIC but lower than those of ZirCAD. Notably, the EXP hardness closely mimics that of the human enamel. The wear volume, SBS, and water sorption/solubility of EXP are comparable to those of CERASMART and ENAMIC. Therefore, EXP has potential applications as a tooth restorative material. [ABSTRACT FROM AUTHOR]