TiO2-ZnO nanocomposites with a constant Ti:Zn molar ratio of 1:0.1 were prepared via sol-gel process followed by calcination at 300, 400, 500, 600, and 700 degrees C. The structural and compositional characterizations of these nanocomposites were performed through XRD, FTIR, SEM, and EDAX. Bandgap was measured using DRS. Photocatalytic performance of the nanocomposites was evaluated by decolorization of methyl orange dye under UV and visible irradiation with and without aeration. The results showed that increase in calcination temperature resulted in nanocomposites with well-defined morphology. Although the particle size increased with increase in calcination temperature, the crystallinity of the particles also increased, resulting in enhanced photocatalytic activity. A temperature-dependent anatase-to-rutile phase transformation was observed in TiO2-ZnO nanocomposite beyond 600 degrees C. The calcination temperature influenced both dye adsorption on the nanocomposites and also dye decolorization by photocatalysis. Even when present at low molar concentration, ZnO in the nanocomposite caused sufficient decrease in bandgap (2.6 eV) at temperatures as low as 400 degrees C, such that visible irradiation could cause dye decolorization. However, the best decolorization performance was observed in the presence of the nanocomposite calcined at 600 degrees C. Aerated systems showed better performance in all cases. Desorption of the dye remaining adsorbed on the nanocomposite at the end of the photocatalytic reaction, confirmed that adsorption accounted for only 6.6 and 3% of dye removal in the nanocomposites calcined at 600 degrees C with UV and visible irradiation, respectively. However, in other systems, ignoring adsorption may cause significant overestimation in photocatalytic loss of dye from the system.