The TiO2 anodized films generated at low current density after annealing are good candidates for surface coating, as a hydrophilicity is a crucial characteristic that determines dental implant applications. In this study, the hydrophilicity of TiO2 anodized films annealed at various temperatures was examined. It was found that increasing the annealing temperature during the anodization procedure improves the hydrophilicity of the TiO2 anodized films. This is related to the evolution of the TiO2 anodized film structure produced by raising the annealing temperature, which converts the TiO2 anodized amorphous phase to rutile phases. Moreover, increased annealing temperature results in more oxygen vacancies, hydroxyl groups, and roughness, which further improves hydrophilicity.