Zirconia dental implants require excellent biocompatibility and high bonding strength. In this study, we attempted to fabricate biocompatible zirconia ceramics through surface modification by hydroxyapatite (HA) slurry coating. A hydroxyapatite slurry for spin coating was prepared using two sizes of hydroxyapatite particles. The hydroxyapatite slurry was obtained by adjusting the solid loading, pH range, and dispersant content. The surface roughness of the HA-coated layers on the zirconia substrate depended on the change in microstructural evolution and coating thickness. With repeated coating, the coating thickness gradually increased for both small and large particles. The specimen with two coatings had the maximum surface roughness but displayed different values depending on the size of the HA particles. High surface roughness (Ra; 0.49 μm) could be obtained from the slurry of small particles compared with that of the large particles (Ra; 0.35 μm). During a 14 days in vitro experiment in SBF solution at pH 7.4, no changes were observed in the surface microstructure of the HA coating layer on the zirconia substrate.