In this study, we present a novel coating with Zn-releasing ability that promotes osseointegration of Ti6Al4V implants. The coatings were prepared by a sol–gel technique, and nanosized Zn-containing β-tricalcium phosphate particles were added to the Ca(NO3)2–P2O5–HPF6 sol system to incorporate Zn ions into fluoridated hydroxyapatite (FHA) coatings. The derived Zn-releasing fluoridated hydroxyapatite (ZTFHA) coatings demonstrated a slow and sustained Zn release behavior. The ZTFHA coatings were able to support cell growth of osteoblast-like cell cultures and promoted an obvious increase in cell viability compared with FHA coating alone. The histological analysis of the ZTFHA coating showed direct bonding to bony tissue and significantly higher bone contact than with FHA coating alone. The ZTFHA coating with its slow and sustained Zn release shows promise as a medium for significantly enhancing osseointegration and allowing cementless stable fixation of orthopedic implants.