Binary titania-silica metal oxides (TiO2-SiO2) have preferentially been used as photocatalysts for the degradation of organic contaminants under UV irradiation. Herein we synthesized TiO2-SiO2 aerogel powders with different Si-to-Ti ratios suitable for decolorization of organic pollutants using less expensive silica source (sodium silicate) and titanium oxychloride as a titania precursor. Consequently, the surfaces of the alcogels were hydrophobized using trimethylchlorosilane (TMCS) as a silylating agent to yield hydrophobic aerogel powders at ambient pressure drying. The as-prepared samples were calcined at different temperatures ranging from 200 to 1000 degrees C to evaluate the effect of the heat treatment in the microstructure of the aerogels. The physico-chemical properties of the aerogels were examined by XRD, FTIR, XRF, TEM, SEM, N-2 gas physisorption studies, TGA/DTA and diffusive reflectance spectrometry analyses. It was found that calcination temperature is an important factor in improving the porosity and crystallinity of the aerogels however; it has a detrimental effect on the hydrophobicity and photochemical performance of the aerogels. The as-synthesized aerogels were hydrophobic and exhibited the highest activity toward decolorization of methylene blue. The hydrophilic aerogels were obtained after calcination at temperature >= 500 degrees C however; the formed samples possessed lower activities. Hydroxyl radicals ((OH)-O-center dot) detection experiment performed in the presence of the phptocatalysts indicated that the generation of radicals during irradiation increases with increasing illumination time. (C) 2013 Elsevier B.V. All rights reserved.