The TiO2 films were synthesized on Ti substrates by a novel method. Titanium metal was directly oxidized by hydrogen peroxide to generate a rough amorphous film and then hydrothermal process transformed the film to crystalline nanoflower TiO2 film. The obtained film can be modified by calcination with urea and the modified film can keep the nanoflower structure. According to the XPS data, the urea-induced modification is surface-modification rather than N-doping. Compared to the un-modified film, the response scope of the modified film extends to the visible light region. Photocatalytic activity of films were investigated by degrading methyl orange (MO) under visible light. As a result, 47% of MO was decomposed by modified film in 3 hours.