Graphite-like carbon deposited single-crystal anatase TiO2 with exposed {001} facets was fabricated through a two-step solvothermal process by using glucose as carbon source. The physicochemical properties of the as-prepared samples were investigated by X-ray diffraction, Brunauer-Emmett-Teller, transmission electron microscopy, Raman, UV–vis diffuse reflectance spectra, electrochemical impedance spectroscopy and surface photovoltage spectroscopy. These results demonstrated that graphite-like carbon layers were deposited on the surface of TiO2 single-crystal nanosheets with exposed highly reactive {001} facets via the dehydration of glucose during the process of hydrothermal treatment. The loading of the graphite-like carbon layers could effectively extend the light absorption edge of the single-crystal anatase TiO2 nanosheets to visible light region and accelerate the separation of photo-generated electrons and holes, contributing an excellent visible-light driven photocatalytic performance to the graphite-like carbon deposited single-crystal anatase TiO2 nanosheets for the degradation of methyl orange.