Collagen/hydroxyapatite (HA) nanocomposite thin films containing 10, 20, and 30 wt.% HA were prepared on commercially pure titanium substrates by the spin coating of their homogeneous sols. All of the nanocomposite coatings having a thickness of ∼7.5 μm exhibited a uniform and dense surface, without any obvious aggregation of the HA particles. A minimum contact angle of 36.5° was obtained at 20 wt.% HA, suggesting that these coatings would exhibit the best hydrophilicity. The in vitro cellular assays revealed that the coating treatment of the Ti substrates favored the adhesion of osteoblast-like cells and significantly enhanced the cell proliferation rate. The cells on the nanocomposite coatings expressed much higher alkaline phosphatase (ALP) levels than those on the uncoated Ti substrates. Increasing the amount of HA resulted in a gradual improvement in the ALP activity. The nanocomposite coatings on Ti substrates also exhibited much better cell proliferation behaviors and osteogenic potentials than the conventional composite coatings with equivalent compositions, demonstrating the greater potential of the former as implant materials for hard tissue engineering.