A series of Fe-ions modified BiOBr photocatalysts were synthesized via a facile solvothermal method. The photocatalysts were characterized by X-ray diffraction, X-ray photoelectron spectroscopy, Fourier transformed infrared spectroscopy, scanning electron microscopy, transmission electron microscopy, N-2-sorption, photoluminescence spectra, and UV-Vis diffuse reflectance spectroscopy. The photocatalytic activities of Fe ions modified BiOBr samples were evaluated by the decomposition of methyl orange under visible light irradiation. The results revealed that the introduction of Fe ions greatly improved the photocatalytic performance of BiOBr. The highest activity was obtained by 15 at.%Fe-BiOBr sample. The reasons for the enhanced photocatalytic activities of Fe ions modified BiOBr samples were attributed to strong photoadsorption in the visible light region, high specific surface area, more chemisorbed water and hydroxyl groups and the mediating role of Fe3+ ions in charge transfer.