Carbon-modified TiO2 was successfully prepared via simple heat treatment of TiO2 in alcohol vapors (1-butanol and 2-butanol) at a constant temperature (500 °C). The prepared samples were characterized by means of X-ray diffraction (XRD) and Fourier transform infrared diffuse reflectance spectroscopy (FTIR/DRS). Brunauer-Emmett-Teller (BET) adsorption and zeta potential analyses were also conducted. The Freundlich adsorption model fitted both carbon-modified and original TiO2, which provide a heterogeneous surface for the adsorption of Orange II. The carbon-modified TiO2 was used as a photocatalyst to remove Orange II from aqueous solution by combined processes of adsorption and photocatalytic decomposition. The adsorption performance of the carbon-modified TiO2 was higher than that of the unmodified TiO2. Carbon adsorption approached synchronicity with oxidation, leading to the higher activity. This enhanced adsorption capacity may be a promising factor for the photocatalytic removal of Orange II onto carbon-modified TiO2. The prepared Carbon-modified TiO2 samples had higher BET surface area than unmodified TiO2 (44, 54.48 and 49.72 m2/g for TiO2, C1B-TiO2 and C2B-TiO2, respectively) and exhibited higher hydrophobicity and a positively charged surface, which were favorable for adsorption of Orange II. High adsorption of dye on the porous structure of C-TiO2 enhanced its photocatalytic decomposition under visible light.