Novel Fe-incorporated anatase TiO2 nanosheet hierarchical spheres with predominant {001} facets were first prepared via a facile one-pot solvothermal route. The obtained {001}-0.1%Fe-AHSs exhibit excellent visible light photodegradation activity for methylene blue attributed to 94% {001} facets and uniformly incorporated Fe3+ ions in the TiO2 lattice.