IR laser- and UV laser-induced ablation of titanium monoxide (TM) in hydrogen (50Torr) is compared to the same process induced in vacuum and shown to result in deposition of hydrated surface modified nanostructured titanium suboxide films. Complementary analyses of the films deposited in vacuum and in hydrogen by Fourier transform infrared, Raman and X-ray photoelectron spectroscopy, X-ray diffraction and electron microscopy allowed to determine different features of both films and propose a mechanism of surface modification of ejected particles, which involves hydrothermal reduction of TM and subsequent reactions of evolved water. The films exert good adhesion to metal and quartz surfaces and are hydrophobic in spite of having their surface coated with adsorbed water.