Three differently treated titanium substrates to be used in dental implant applications and with different surficial morphology were coated with titanium dioxide (TiO2) films by using Low-Pressure Metal Organic Chemical Vapor Deposition (MOCVD). No literature references were found on the performance evaluation of the TiO2 MOCVD coatings on substrates with different pristine morphology; in this work the influence of the pristine Ti surface characteristics on TiO2 crystalline structure, morphology, wettability as well as on ion release, electrochemical behavior, tribocorrosion performance, and nano-mechanical properties were studied and discussed. It was shown that the pristine substrate influenced both the crystalline phases' formation and crystallite size. Scanning electron microscopy analyses and roughness evaluation showed the optimal conformal coverage of all the MOCVD coatings for all substrates, with grain size depending on the substrate morphology and topography. The wettability of the TiO2 coated Ti substrates highlighted a superhydrophilic behavior and, if stored in air, decreased as a function of the time aging. Ions release tests, nanoindentation measurements, tribocorrosion, and potentiodynamic polarization experiments suggest the enhancement of functional properties of the coated samples. Titania sandblasted/acid etched coated Ti substrates generally showed the best performance of the functional properties for their use in dental implant fabrications.