Octadecyltrichlorosilane (OTS) was grafted on titanium using self-assembly technique, after UV irradiation, its hydrophobic nature was changing. The calcium phosphate coatings was tunablely prepared by electrochemical deposition on functionalized titanium surface with different experiment conditions. The correlative structure and morphology of CaP coatings on titanium were characterized by X-ray diffractometer (XRD), field emission scanning electron microscope (FE-SEM) and transmission electron microscope (TEM) under the preparation parameters. Its grain size under different conditions was calculated by Scherrer formula. The results indicated that the morphology of CaP coatings under different conditions were significant difference, and the grain sizes were ranged 12.46nm from 190.1nm. The study demonstrated that OTS functionalized titanium surface could be a controllable preparation of uniform and orderly nano CaP coatings, which is expected to improve the biocompatibility of implant materials.