Carbon quantum dots/TiO2 nanosheets with a majority of (001) facet (CQDs/TiO2-001) samples are successfully prepared via a facile method. Compared to TiO2-001 and CQDs/P25, the synthesized CQDs/TiO2-001 presents a remarkably higher photocatalytic activity for H-2 evolution with a considerable stability. XRD, XPS, HRTEM, FESEM, FTIR, Photoluminescence (PL) spectroscopy, Fluorescence spectroscopy and UV-visible reflectance spectroscopy are adopted to investigate the morphology, structure and properties of synthesized CQDs/TiO2-001. The mechanism of the improved photocatalytic activity over CQDs/TiO2-001 is also investigated. The results show that the improved photocatalytic activity over CQDs/TiO2-001 can be attributed to the synergistic effects of TiO2-001 and CQDs: the highly exposed (001) facets of TiO2-001 promote the transportation of photogenerated electrons and the loading of CQDs restrains the recombination of electrons-holes on (001) facets. Meanwhile, the visible-light absorption is extended because the CQDs serve as a photosensitizer and sensitize TiO2-001 through the newly formed Ti-O-C bond between the CQDs and TiO2-001.