Surface titanium (Ti) metallization was conducted on alumina (AlO) through chemical vapor deposition (CVD) method derived from non-contact pack cementation. The effects of different deposition temperature (1000 °C, 1050 °C, and 1100 °C) were examined in this scenario. The morphology, phase composition, and interfacial defects of the resulting films were systematically investigated through scanning electron microscopy, energy dispersive spectrometry, and X-ray diffraction. The nanomechanical characterization of the proposed thin films was evaluated by conducting nano-indentation tests at different depths. The results revealed that uniform Ti films were coated on the AlO substrate. During coating, the atoms on the matrix surface were driven to form different structure due to different deposition temperature, leading to disparate morphologies of the surface and the interface, which consequently influenced the binding force between the film and the substrate. Moreover, the nanomechanical properties were found to be related to the internal and interface structure. Decreased modulus and hardness were obtained for metallization films treated at 1050 °C, and plastic deformation was the main deformation pattern.