Oxyapatite, amorphous calcium phosphate, and double-layered calcium phosphate coating films were fabricated on mirror-polished commercially pure titanium (CP Ti) and blasted Ti-6Al-4V alloy substrates by radiofrequency (RF) magnetron sputtering; the properties of these films were evaluated in vivo and in vitro. The bonding strength between the calcium phosphate films and the Ti substrates was higher than 50 MPa. This value is higher than the bonding strength reported in the case of plasma-sprayed calcium phosphate coating films fabricated on Ti substrates. The removal torque of screw-type blasted Ti-6Al-4V alloy implants in the femurs of Japanese white rabbits increased with the duration of implantation, and the removal torque values of the coated implants was observed to be higher than those of the non-coated implants. In vitro and in vivo studies indicate that coating Ti implants with calcium phosphate films using RF magnetron sputtering is effective in improving the bone compatibility of Ti implants. Finally, the factors that should be considered in fabricating biomedical coating films were discussed.