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Introducing polarization field of piezoelectric materials is an effective strategy to improve photocatalytic performance. In this study, a new type of BaTiO3/CuO heterostructure catalyst was designed and synthesized to achieve high piezo-photocatalytic activity through the synergy of heterojunction and piezoelectric effect. The BaTiO3/CuO heterostructure shows a significantly enhanced piezo-photocatalytic degradation efficiency of organic pollutants compared with the individual BaTiO3 nanowires (NWs) and CuO nanoparticles (NPs). Under the co-excitation of ultrasonic vibration and ultraviolet radiation, the optimal degradation reaction rate constant k of polarized BaTiO3/CuO heterostructure on methyl orange (MO) dye can reach 0.05 min−1, which is 6.1 times of photocatalytic rate and 7 times of piezocatalytic rate. The BaTiO3/CuO heterostructure with remarkable piezo-photocatalytic behavior provides a promising strategy for the development of high-efficiency catalysts for wastewater purification, and it also helps understand the coupling mechanism between piezoelectric effect and photocatalysis.