This paper describes efforts to improve implant biocompatibility and durability by applying a hybrid technique using composite oxidation. Pure titanium was used as the substrate material. A porous oxide film as the outer layer was produced by micro-arc oxidation and a dense oxide film as the inner layer was produced by pre-anodic oxidation. In this study, physicochemical characteristics, corrosion test, cell attachment behavior, and in vivo studies were used to compare this gradient layer with untreated titanium. The results revealed that the gradient layer was composed of two layers of oxide films which were made up of rutile and anatase and the surface was porous with calcium and phosphor. The corrosion resistance of the gradient layer was improved remarkably, which was about three times the values for titanium and two times the value for the dense layer. The cell-material interaction study indicated that L929 cells seeded and cultured on the gradient layer appeared to attach well and the rate of proliferation was the greatest. The study in vivo showed that the gradient layer had good biocompatibility. This gradient layer provides a material with high corrosion resistance, bioactivity, and biological properties suitable for tissue engineering applications.