Fe,F co-doped TiO2 nanotubes (Fe,F/TiO2 NTs) were synthesised by the combination of hydrothermal process and impregnation method. The structure and composition of prepared catalysts were investigated by X-ray diffraction (XRD), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). XRD results confirmed only the presence of the anatase phase in Fe,F/TiO2 NTs. Well-defined TiO2 NTs with nearly uniform diameters could be seen from the TEM images. Also, the high-resolution XPS spectra of Fe 2P and F 1s showed that Fe3+ and F− existed in TiO2 lattice and on the surface of TiO2, respectively. The photocatalytic performances of Fe/TiO2 NTs and Fe,F/TiO2 NTs with different Fe concentrations were evaluated by photo-degrading aqueous methyl orange under visible light irradiation, and the results showed that the photoactivity of Fe and F co-doped TiO2 NTs was enhanced obviously compared with Fe mono-doped TiO2 NTs and the 0.5% Fe,F/TiO2 NTs presented the best photocatalytic performance.