Although zirconia ceramics were highly versatile as dental implants, their long-term presence in the human body may slow down healing and impede cell growth in the past. To enhance the cytocompatibility of zirconia ceramics, surface activation modification was used to immobilize biopolymers such that a biomimetic environment was created. Hexamethyldisilazane thin films were deposited onto the surface of inorganic zirconia through cold plasma treatment under various power and deposition time settings to form an organosilane interface layer. Next, oxygen plasma treatment was performed to activate the free radicals on the surface. Subsequently, ultraviolet light was employed to graft and polymerize acrylic acid for generating carboxyl groups on the surface. This was followed by a condensation reaction with biopolymers (chitosan, chitosan/poly-γ-glutamic acid, and gelatin). Under a 20-min deposition time at 40W and 150 mTorr, the thin films had a maximum graft density of 2.1mg/cm2. MG-63cells (human osteosarcoma cells) were employed to evaluate cell compatibility. Chitosan and chitosan/poly-γ-glutamic acid promoted the compatibility of MG-63cells (a human osteosarcoma cell line) with zirconia ceramics, whereas gelatin reduced this compatibility. The findings confirm that cold plasma treatment and graft polymerization can promote the immobilization of biomolecules and improve the biocompatibility of zirconia ceramics. This approach can be applied to the modification of zirconia ceramic implants.