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Layer-by-layer self-assembled TiO2hierarchical nanosheets with exposed {001} facets have been successfully fabricated via a simple one-step solvothermal reaction. The anatase TiO2layer-by-layer hierarchical nanosheets (TiO2LHNs) exhibit favorable light scattering effect and large surface area, owing to their layer-by-layer hierarchical structure. When applied to the dye-sensitized solar cells (DSSCs), the layer-by-layer hierarchical structure with exposed {001} facet could effectively enhance light harvesting and dye adsorption, followed by increasing the photocurrent of DSSCs. As a result, the photoelectric conversion efficiency (η) of 7.70% has been achieved for the DSSCs using TiO2LHNs as the bifunctional layer, indicating 21% improvement compared to the pure Degussa P25 (6.37%) as photoanode. Such enhancement can be mainly ascribed to the better light scattering capability of TiO2LHNs, higher dye adsorption on TiO2LHN {001} facets, and longer lifetime of the injected electrons in TiO2LHNs compared to P25, which are examined by UV–vis spectrophotometry and electrochemical impedance spectroscopy under the same conditions. These remarkable properties of TiO2LHNs make it a promising candidate as a bifunctional scattering material for DSSCs.