Fe-doped titanate nanotubes were prepared by the combination of sol–gel process with hydrothermal treatment. After a further calcinations process, Fe-doped TiO2 nanotubes (Fe/TiO2 NTs) with high photocatalytic activity were obtained. The prepared catalysts were characterized by XRD, TEM, and XPS. The photocatlytic activity of Fe/TiO2 NTs was evaluated through the photodegradation of aqueous methyl orange. The experiments demonstrated that the 0.5% Fe/TiO2 NTs calcined at 300 °C possessed the best photocatalytic activity. Compared with pure TiO2 nanotubes, the doping with Fe significantly enhanced the photocatalytic efficiency.