Ordered 2-D hexagonal mesoporous TiO2-SiO2 nanocomposites consisted of anatase TiO2 nanocrystals and amorphous SiO2 nanoparticles, with large mesochannels and high specific surface areas, have been extensively and detailedly evaluated using various cationic dyes (methylene blue, safranin O, crystal violet, brilliant green, basic fuchsin and rhodamine-6G), anionic dyes (acid fuchsin, orange II. reactive brilliant red X3B and acid red 1) and microcystin-LR. We use mesoporous 80TiO(2)-20SiO(2)-900 for the degradation of cationic dyes and MC-LR, due to the dominant adsorption of Si-OH groups and synergistic role of coupled adsorption and photocatalytic oxidation. For anionic dyes, due to the adsorption results predominantly from Ti-OH groups, our strategy realizes the enhanced photocatalytic oxidation by strong surface acids and larger available specific surface area. Based on this, we prepared 90TiO(2)-10SiO(2)-700 to degrade them. The results show that our samples exhibit excellent degradation activities to all the contaminants, which are much higher than that of P25 photocatalyst. The dyes are not only decolorized promptly but degraded readily as well. It is strongly indicated that our mesoporous nanocomposites are considerably stable and reusable. These results demonstrate that our mesoporous TiO2-SiO2 nanocomposites present extensive and promising application in the fast and highly efficient degradation of various organic pollutants. (C) 2012 Elsevier B.V. All rights reserved.