In this work, commercial anatase TiO 2 powders were modified using ultrathin Fe 2 o 3 layer by atomic layer deposition (ALD). The ultrathin Fe 2 o 3 coating having small bandgap of 2.20 eV can increase the visible light absorption of tio 2 supports, at the meantime, Fe 2 o 3 /tio 2 heterojunction can effectively improve the lifetime of photogenerated electron-hole pairs. Results of ALD Fe 2 o 3 modified TiO 2 catalyst, therefore, showed great visible light driven catalytic degradation of methyl orange compared to pristine tio 2. A 400 cycles of ALD Fe 2 o 3 (~ 2.6 nm) coated TiO 2 powders exhibit the highest degradation efficiency of 97.4% in 90 min, much higher than pristine TiO 2 powders of only 12.5%. Moreover, an ultrathin ALD Al 2 o 3 (~ 2 nm) was able to improve the stability of Fe 2 o 3-tio 2 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. A rapid industrial development driven by unsustainable technology advances can cause plenty of industrial sewage, spreading chemical hazards into water resources. As a result, water pollution has emerged as one of the most serious environmental issues worldwide 1-4. Photocatalytic oxidation technology has shown great prospects in removing the toxic and harmful contaminants in aqueous environment 5-7. Semiconductors (e.g. TiO 2 , ZnO, SnO 2) have been widely researched for organic pollutant degradation, however, the large band gap hinders their practical applications 8-12. For example, TiO 2 with band gap of 3.2 eV can only absorb the ultraviolet light, accounting for only 4-5% of entire solar spectrum 13. Therefore, various visible light sensitive photocatalysts has also been widely explored, such as g-C 3 N 4 , BiVO 4 , CdSe, Bi 2 WO 6 14-19. On the other hand, TiO 2 is recognized as one of the excellent materials owning to its good inertness, eco-friendly, low cost, strong oxidizing power, and long-term stability against photo and chemical corrosion 9,13,20-22. Thus, plenty of works have been made to extend the absorption spectrum of TiO 2 to visible light so to make a full use of solar spectrum. Several different approaches can be employed, including doping 23-26 and coupling with small band gap semiconductors or metals 27-30. Small band gap semiconductors not only increase the absorption of visible light but also inhibit photogenerated electrons-holes recombination when constructed as a semiconductor/semiconductor heterojunction structure, thus improving the photocatalytic performance dramatically 31. Therefore, various TiO 2 based heterojunction photocatalysts have been proposed for visible light photocatalysis, including NiO/TiO 2 32,33