In this work, commercial anatase TiO2 powders were modified using ultrathin Fe2O3 layer by atomic layer deposition (ALD). The ultrathin Fe2O3 coating having small bandgap of 2.20 eV can increase the visible light absorption of TiO2 supports, at the meantime, Fe2O3/TiO2 heterojunction can effectively improve the lifetime of photogenerated electron-hole pairs. Results of ALD Fe2O3 modified TiO2 catalyst, therefore, showed great visible light driven catalytic degradation of methyl orange compared to pristine TiO2. A 400 cycles of ALD Fe2O3 (~ 2.6 nm) coated TiO2 powders exhibit the highest degradation efficiency of 97.4% in 90 min, much higher than pristine TiO2 powders of only 12.5%. Moreover, an ultrathin ALD Al2O3 (~ 2 nm) was able to improve the stability of Fe2O3-TiO2 catalyst. These results demonstrate that ALD surface modification with ultrathin coating is an extremely powerful route for the applications in constructing efficient and stable photocatalysts.