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Abstract Hierarchical Bi2Fe4O9/BiOI S-scheme nanoflower heterostructures are prepared by hydrothermal method, which exhibit exceptional photo-piezoelectric catalytic performance. The tight binding between the sheets ensures the efficient electron transport, and provides a large interface area and adequate reaction sites for photo-piezoelectric catalytic reactions. At the same time, because the water flow in the water body produces hydraulic shear force on the material, the material produces piezoelectric effect. Bi2Fe4O9/BiOI exhibit a remarkable degradation efficiency of 99.4% for tetracycline and a hydrogen production rate of 4089.36 µmol h−1 g−1. The observed behavior can be explained by the combined influence of the formation of S-scheme structure and the process of photo-piezoelectric catalysis, confirmed by in-situ XPS, transient/steady-state fluorescence and piezoelectric response force test. The excellent stability of the material suggests its possible use in the sectors of energy and environment. This work introduces novel concepts for the future advancement of photo-piezoelectric synergistic catalysis.