Extending the response range of wide-bandgap (3.2 eV) anatase TiO2 photocatalysts into the visible light range can play an important role in promoting the practical applications of photocatalysts. Here, we report a route to prepare sulfur doped anatase TiO2 single crystal sheets with a high percentage of (0 0 1) facets. The resultant TiO2 sheets were investigated by a combination of experimental characterizations and electronic structure calculations. The synthesized sulfur doped anatase samples show an additional visible light absorption band from 400 nm to ca. 550 nm and some visible-light photocatalytic activity in (OH)-O-center dot radical generation and photodecomposition of organic dyes. The Ti-S bond structure causes not only visible light absorption but also changes to an extent the surface structures of doped anatase TiO2 sheets. Theoretically, localized 3p states of S formed in the bandgap are implicated for the visible light absorption of the sulfur doped anatase TiO2. (C) 2010 Elsevier Inc. All rights reserved.