A one-step and room-temperature process for depositing nanoparticles or nanocomposite (nanoparticle-assembled) films of metal oxides such as crystalline titanium dioxide (TiO2) onto a substrate surface using ultrafast pulsed laser ablation of Titania or metal titanium target. The system includes a pulsed laser with a pulse duration ranging from a few femtoseconds to a few tens of picoseconds, an optical setup for processing the laser beam such that the beam is focused onto the target surface with an appropriate average energy density and an appropriate energy density distribution, and a vacuum chamber in which the target and the substrate are installed and background gases and their pressures are appropriately adjusted.