Yellow–colored pure titania with a mesoporous structure was prepared by the aggregate of titania nanocrystals, which were stabilized by exfoliated titanate nanosheets via an electrostatic interaction. X–ray diffraction patterns and images of transmission electron microscope confirm that titanate sheets are randomly dispersed into the assembled titania nanocrystals without forming any self–restacked phase. This nanocrystals–nanosheets composite exhibits a mesoporous structure with pore size of ~ 6.5 nm and surface area of 236.3 m2 g− 1. Greatly different from the UV–responded properties of titania nanocrystals and titanate nanosheets, the absorption edge of nanocomposite red–shifts to visible light region. The visible light photocatalytic tests demonstrate that this nanocomposited titania shows excellent activity for the degradation of organic dyes, as well as a colorless organic pollutant of 2, 4–dichlorophenol. The possible photocatalytic mechanism that photogenerated holes as the mainly oxidant species in photocatalysis is proposed based on the trapping experiments of hydroxyl radicals or photogenerated holes. Moreover, as the nanocomposite depicts an extreme stability, no obvious deactivation occurs after five cycles.