Two kinds of aluminum-based titania nanocomposites, TiO2-boehmite (TiO2-AlOOH) and TiO2-alumina (TiO2-Al2O3), were fabricated into a commercially available titania via the direct condensation of aluminum tri-sec-butoxide and P25in this investigation. As synthesized samples were structurally characterized by Fourier transform-infrared spectrophotometer (FT-IR), X-ray diffraction (XRD), nitrogen physisorption, and scanning electron microscopy (SEM). It was confirmed that titania was incorporated into the aluminum matrixes to form nanocomposites, the photocatalytic efficiency were further measured by using methylene blue (MB) as a simulation pollutant. Moderate decolorization efficiency of TiO2-Al2O3was found, while much higher decolonization efficiency of TiO2-boehmite was observed, possibly attributing to the larger surface area with the presence of abundant hydroxyl groups. In addition, the best decolorization efficiency of both composites was found under alkaline condition.