In order to obtain TiO2 with high photocatalytic activity, a cathode reduction was used to dope I7+ and I5+ into TiO2 nanotubes of anodized Ti in C2H2O4 · 2H2O + NH4F electrolyte. SEM images show that the anodization method integrated the preparation with the doping process, which for nonmetals-doping is advantageous to maintain the morphological integrity of TiO2 nanotubes. I7+-I5+-doping enhances the UV response of TiO2 and result in a red-shift. Under UV/visible irradiation, a I7+-I5+-doped sample (400°C) showed the highest I ph and photocatalytic efficiency. A part of I− in the I7+-I5+-doped sample is involved in the UV response, the red-shift and the higher I ph.