The β-titanium alloy is thought to be a promising alloy using as orthopedic or dental implants owing to its characteristics, which contains low elastic modulus, high corrosion resistance and well biocompatibility. Our previous study has reported that a new β-titanium alloy Ti35Nb2Ta3Zr showed low modulus close to human bone, equal tissue compatibility to a traditional implant alloy Ti6Al4V. In this study, micro-arc oxidation (MAO) was applied on the Ti35Nb2Ta3Zr alloy to enhance its surface characteristics and biocompatibility and osseointegration ability. Two different coatings were formed, TiO2 doped with calcium-phosphate coating (Ca-P) and calcium-phosphate-strontium coating (Ca-P-Sr). Then we evaluated the effects of the MAO coatings on the Ti35Nb2Ta3Zr alloy through in vitro and in vivo tests. As to the characteristics of the coatings, the morphology, chemical composition, surface roughness and contact angle of MAO coatings were tested by scanning electron microscopy, energy dispersive spectroscopy, atomic force microscopy, and video contact-angle measurement system respectively. Besides, we performed MTT assay, ALP test and cell morphology-adhesion test on materials to evaluate the MAOed coating materials' biocompatibility in vitro. The in vivo experiment was performed through rabbit model. Alloys were implanted into rabbits' femur shafts, then we performed micro-CT, histological and sequential fluorescent labeling analysis to evaluate implants' osseointegration ability in vivo. Finally, the Ca-P specimens and Ca-P-Sr specimens exhibited a significant enhancement in surface roughness, hydrophilicity, cell proliferation, cell adhesion. More new bone was found around the Ca-P-Sr coated alloy than Ca-P coated alloy and Ti35Nb2Ta3Zr alloy. In conclusion, the MAO treatment improved in vitro and in vivo performance of Ti35Nb2Ta3Zr alloy. The Ca-P-Sr coating may be a promising modified surface formed by MAO for the novel β-titanium alloy Ti35Nb2Ta3Zr.