Fe3+ doped together with Au deposited TiO2 (Au/Fe3+-TiO2) was successfully prepared, which shows excellent photocatalytic activity for degradation of methyl orange (MO) under both UV and visible light (lambda > 420 nm) illumination. Fe3+ has been confirmed by EPR to substitute for Ti4+ in the TiO2 lattice, and Au exists as Au-0 on the surface of the photocatalyst indicated by the results of XRD. Fe3+ and Au have synergistic effects on improving the photocatalytic activity of TiO2. A proposed mechanism concerning the synergistic effects is discussed to explain the improvement of the photocatalytic activities.