In this article, an ordered two-dimensional (2D) hexagonal mesoporous anatase crystals-silica nanocomposite was first synthesized using synchronous-assembly of surfactant and inorganic precursors molecules, and then a three-dimensional (3D) interconnected mesoporous anatase TiO2 was prepared via an "extracting silica" approach. The results show that the mesopore channels in our titania are highly connected by plenty of 3D uniform intrawall mesopores while retaining mesostructural integrity and regularity. The TiO2 prepared is completely anatase crystalline with uniform nanocrystals (13.0 nm in size) and a high specific surface area (similar to 145 m(2)/g). This method is mild, simple and can be easily repeatable. The photocatalytic degradation rates of Acid Red 1 (0.173 min(-1)) and microcystin-LR (2.57 min(-1)) on the interconnected mesoporous TiO2 are very high, which are 41.6 and 2.85 times higher than that of the parent sample; 29.2 and 7.20 times that of P25 photocatalyst, respectively. These results clearly demonstrated that the 3D interconnected mesostructure played a key role in the activity increments. In addition, our photocatalysts are considerably stable and reusable. To the best of our knowledge, such results have not been seen in the literature before. Furthermore, the fundamentals of this study would provide new insights for the rational design and preparation of 3D highly interlinked mesoporous metal-oxides with unique photocatalytic performances. (C) 2017 Elsevier B.V. All rights reserved.