In order to expand the family and improve the bioactivity of oral implant ceramics, the phase structures, mechanical and wetting properties of the hot-pressed yttria-zirconia/multilayer graphene oxide composite (3Y-ZrO2/GO) ceramics were investigated. GO was uniformly distributed in 3Y-ZrO2 powders, forming the C–O–Zr bond during the sintering process. In comparison to raw 3Y-ZrO2 ceramics, the flexural strength and fracture toughness improved up to 200% (1489.96 ± 35.71 MPa) in ZG3 (with 0.15 wt% GO) and 40.9% (8.95 ± 0.59 MPa m1/2) in ZG2 (with 0.1 wt% GO), respectively, while the relative density and Vickers hardness increased slightly. The toughening mechanisms included crack deflection, crack bridging, and GO put-out. Meanwhile, the composite ceramics were transformed into a more hydrophilic direction and indicated a good wetting property. In consideration of mechanical and wetting properties, the ZG3 would be a favorable alternative to the yttria-zirconia ceramic (Y-TZP) in dental implant applications. The results are expected to serve as a technical guidance for the fabrication and evaluation of dental implants.