〔Abstract〕 Objective. , To evaluate the mechanical properties and biocompatibility of a 3 mol% yttria-stabilized tetragonal zirconia polycrystal (3Y-TZP)-polymethyl methacrylate (PMMA) biomimetic layered composite and to explore the feasibility of using this composite for ceramic dental crowns. Methods The micro-morphology of 3Y-TZP powder was observed using scanning electron microscopy and metallographic microscopy. The ball-milled 3Y-TZP powder was stirred together with bacterial cellulose to obtain a homogeneous ceramic slurry. Uniform ceramic films were prepared by tape casting. After stacking the ceramic films, the composite was finally obtained through pressure-less sintering, silane coupling, and organic matter infiltration. The microstructure of the composite was observed using scanning electron microscopy. The mechanical properties of the composite were measured using a universal testing machine, and the energy dissipation rate and impact toughness of the samples were evaluated through ball drop and falling weight impact tests. The biocompatibility of the composite was investigated using CCK-8 assay, live/dead cell staining, cell adhesion assay, and Transwell cell migration assay. Results The composite exhibited a distinct layered structure. As the thickness of the ceramic layer decreased, the bending and compressive strengths of the material gradually decreased, while its impact resistance was significantly improved. The maximum energy dissipation rate and impact toughness can reach 75.8% and 44.1 kJ/m²respectively. No significant differences were observed in the CCK-8 assay, live/dead cell staining, or cell migration assay results between the blank group and the material group, and cells were able to adhere well to the composite. Conclusion This study successfully fabricates 3Y-TZP-PMMA composite materials, which possess both excellent mechanical properties and biocompatibility, demonstrating promising prospects for clinical application.