Biocompatibility and osteointegration of implants are highly desired in orthopedic and dentistry applications. The synthesis of a coating with ideal biocompatibility and osteogenic effect carries practical significance for improving the bio-inertness of pure Ti implants. Metal-organic frameworks (MOFs) are effective surface modification agents in bone regeneration applications. Bio-MOF-1, a classic type of biofriendly MOF with a bio-derived constitution, possesses biocompatibility and osteogenic potential resulting from its Zn core and adenine ligand. In this study, bio-MOF-1 coatings at multiple concentrations were synthesized on alkali-heat treated Ti, and their cytocompatibility and osteogenic properties were systematically examined both in vitro and in vivo. Coatings were characterized to confirm the successful synthesis of bio-MOF-1 coatings. These coatings exhibited advanced thermostability, excellent biocompatibility, and stable Zn2+ release, which up-regulated the expression of osteogenesis-related genes and proteins. Furthermore, bio-MOF-1 coating of Ti implants enhanced early osseointegration at the bone-implant interface. This study demonstrates the promising potential of bio-MOF-1 coatings with the osteogenic effect for surface modification in bone tissue engineering.