The nano-hydroxyapatite/zirconia coating of double layers on surface of titanium allay materials have been prepared using electrochemical method. The features and structures of the composite coating materials are studied and analyzed by the Scanning electron microscope (SEM) and EDAX measurement. The results show that nano-HA/ZrO2 are densely and uniformly deposited on the surface of titanium allays in ionic form, a stable gradient composite coating, in which the nano-zirconium oxides (ZrO2) are homogeneously distributed between HA and titanium surfaces, are obtained. The tensile strength experiment exhibits that the adhesion or combined strength of the coating with the titanium surface is higher and about 17GPa, which manifests the nano-HA/ ZrO2 coating is successfully combined on the surface of the titanium allay materials. The biological experiments represent that this material can be used in repairing of bone and medical dental- implant of teeth.