Improving fracture toughness, electrical conductivity, and biocompatibility has consistently presented challenges in the development of artificial bone replacement materials. This paper presents a new strategy for creating high-performance, multifunctional composite ceramic materials by doping graphene oxide (GO), which is known to induce osteoblast differentiation and enhance cell adhesion and proliferation into barium calcium zirconate titanate (BCZT) ceramics that already exhibit good mechanical properties, piezoelectric effects, and low cytotoxicity. Using fast hot-pressed sintering under vacuum conditions, (1 − x)(Ba0.85Ca0.15Zr0.1Ti0.9)O3−xGO (0.2 mol% ≤ x ≤ 0.5 mol%) composite piezoelectric ceramics were successfully synthesized. Experimental results revealed that these composite ceramics exhibited high piezoelectric properties (d33 = 18 pC/N, kp = 62%) and microhardness (173.76 HV0.5), meeting the standards for artificial bone substitutes. Furthermore, the incorporation of graphene oxide significantly reduced the water contact angle and enhanced their wettability. Cell viability tests using Cell Counting Kit-8, alkaline phosphatase staining, and DAPI staining demonstrated that the GO/BCZT composite ceramics were non-cytotoxic and effectively promoted cell proliferation and growth, indicating excellent biocompatibility. Consequently, with their superior mechanical properties, piezoelectric performance, and biocompatibility, GO/BCZT composite ceramics show extensive potential for application in bone defect repair.