We report that mild oxidation of Ti foils in air results in brookite-rich titanium oxide (TiO2) films with similar spectral response to that of dye-sensitized TiO2. X-ray powder diffraction and Raman spectroscopy show that the onset of brookite formation occurs at 500°C, and the material is characterized by a strong absorption band in the visible spectral range. The first-principle calculations show that enhanced visible light absorption correlates with the presence of Ti interstitials. Photocurrent density measurements of water splitting reveal that the brookite-rich TiO2 exhibits the highest photocatalytic performance among the different forms of TiO2 produced by oxidation of Ti foils. With increasing oxidation temperature transformation to the rutile phase accompanied by declining visible range photoactivity is observed.