Third-generation TiO2 photocatalysts were prepared by implantation of C+ ions into 110 nm thick TiO2 films. An accurate structural investigation was performed by Rutherford backscattering spectrometry, secondary ion mass spectrometry, X-ray diffraction, Raman-luminescence spectroscopy, and UV/VIS optical characterization. The C doping locally modified the TiO2 pure films, lowering the band-gap energy from 3.3 eV to a value of 1.8 eV, making the material sensitive to visible light. The synthesized materials are photocatalytically active in the degradation of organic compounds in water under both UV and visible light irradiation, without the help of any additional thermal treatment. These results increase the understanding of the C-doped titanium dioxide, helpful for future environmental applications.