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In the work, visible-light-driven hierarchical Bi 3.84 W 0.16 O 6.24 photocatalysts have been synthesized by a facile hydrothermal strategy. The microstructures and photocatalytic activities of Bi 3.84 W 0.16-O 6.24 photocatalysts were finely tuned just by adjusting the pH values of reaction solutions with different alkalis. The as-prepared samples were physically characterized by X-ray powder diffraction, fieldemission scanning electron microscopy, and ultraviolet-visible diffraction reflection spectroscopy. When evaluated by the photocatalytic degradation of methyl orange (MO) under the visible-light irradiation, Bi 3.84 W 0.16 O 6.24 samples with distinct micro-structures showed different photocatalytic activities. Of Note, the hierarchical Bi 3.84 W 0.16 O 6.24 sub-microspheres constructed by nanoflake building blocks demonstrated the highest photocatalytic activity for the degradation of MO under the visible-light irradiation.