A simple one-pot hydrothermal synthesis route has been employed to fabricate the bismuth-doped (Bi-doped) anatase TiO2 hollow thin sheets with {001} facets exposed. Controlling BiVO4 precursor concentration plays a key role in tuning the morphology and the Bi doping concentration of TiO2 hollow thin sheet catalysts. The photocatalytic activity of as-prepared catalysts was evaluated through the photodegradation of different organic dyes under visible light irradiation (>400 nm), including methylene blue (MB), methyl orange (MO), rhodamine-B (RhB), and p-nitroaniline (PNA). Results showed that the optimal dopant of 0.8 atom % Bi in TiO2 achieved the best photocatalytic activity, especially for possessing a much higher photodegradation of PNA, which could be ascribed to the results of photoinduced charge separation and transfer combined with low bulk recombination of charge carriers. This discussion demonstrates that the design of new TiO2 nanostructures for application in solar energy conversion could be easily achieved by coupling Bi cation-doping and active facets with hollow thin sheet morphology.