In this work, coupling of the hydrogen (H2) production and dye degradation was first realized in a single flexocatalytic process using cerium oxide nanorods (CeO2 NRs). The flexoelectric polarization in a bending nanorod created an internal electric field, which promoted the separation of the thermal-excited electrons and holes. As a consequence, the H2 evolution rate of the flexocatalysis in dark was twice higher than that of the photocatalysis by the same CeO2 NRs. Moreover, simultaneous dye degradation was realized without reducing the H2 evolution rate, with the degradation constant rate of 0.065 min−1, dye removal efficiency of 89.3%, and H2 generation at 486.4 μmol g−1 h−1. The dual-functional catalytic performance of the CeO2 NRs was benefited from the unique periodic flexoelectric field induced by the ultrasound vibration, which could not be achieved by photocatalysis. This work revealed the important role of flexoelectric effect in overcoming the limitation in photocatalysis, which could be extended to a wide range of semiconductor nanomaterials for designing novel kinds of advanced flexocatalysts.