3Y-TZP (3 mol% yttria-stabilized tetragonal zirconia polycrystals) ceramics have excellent mechanical properties including high fracture toughness, good abrasion resistance as well as chemical and biological stability. As a result, they are widely used in mechanical and medical components such as bearings, grinding balls, and hip implants. In addition, they provide excellent light transmittance, biocompatibility, and can match tooth color when used as a dental implant. Recently, given the materials’ resemblance to human teeth, these ceramics have emerged as an alternative to titanium implants. Since the introduction of CAD/CAM in the manufacture of ceramic implants, they’ve been increasingly used for prosthetic restoration where aesthetics and strength are required. In this study, to improve the surface roughness of zirconia implants, we modified the 3YTZP surface with a biocomposite of hydroxyapatite and forsterite using room temperature spray coating methods, and investigated the mixed effect of the two powders on the evolution of surface microstructure, i.e., coating thickness and roughness, and biological interaction during the in vitro test in SBF solution. We compared improvement in bioactivity by observing dissolution and re-precipitation on the specimen surface. From the results of in vitro testing in SBF solution, we confirmed improvement in the bioactivity of the 3Y-TZP substrate after surface modification with a biocomposite of hydroxyapatite and forsterite. Surface dissolution of the coating layer and the precipitation of new hydroxyapatite particles was observed on the modified surface, indicating the improvement in bioactivity of the zirconia substrate.