Titanium dioxide has been widely used in modern industrial applications, especially as an effective photocatalyst. Recently, freestanding TiO2 films with a markedly reduced bandgap of ∼1.8 eV have been synthesized, indicating that the dimension has a considerable influence on the bulk band gap (>∼3 eV) and enhances the adsorption range of visible light. Titanium oxide compounds have various stoichiometries and versatile properties. Therefore, it is very necessary to explore the electronic properties and functionalities of other titanium oxide films with different stoichiometries. Here, we combined structure searches with first-principle calculations to explore candidate Ti-O films with different stoichiometries. In addition to the experimentally synthesized TiO2 film, the structure searches identified three new energetically and dynamically stable Ti-O films with stoichiometries of Ti3O5, Ti3O2, and Ti2O. Calculations show that the Ti-O films undergo several interesting electronic transformations as the Ti fraction increases, namely, from a wide-gap semiconductor (TiO2, 3.2 eV) to a narrow-gap semiconductor (Ti3O5, 1.80 eV) and then to metals (Ti3O2 and Ti2O) due to the abundance of unpaired Ti-d electrons. In addition to the electronic transformations, we observed nonmagnetic (TiO2) to ferromagnetic (Ti3O5, Ti3O2, and Ti2O) transformations. Notably, the Ti3O5 film possesses both narrow-gap semiconductive and ferromagnetic properties, with a large magnetic moment of 2.0 μB per unit cell; therefore, this film has high potential for use in applications such as spintronic devices. The results highlight metal fraction-induced electronic and magnetic transformations in transition metal oxide films and provide an alternative route for the design of new, functional thin-film materials. © 2019 Author(s).