Piezo-modulated interface engineering is an effective method for tuning the charge transfer process to enhance piezocatalytic dynamics. In this study, SrTiO3/ZnO heterojunctions were successfully synthesized via hydrothermal methods to degrade carbamazepine in water. The optimal SrTiO3/ZnO-5 % sample exhibited a remarkable 99.9 % degradation efficiency of carbamazepine within 60 min under ultrasonic vibration. The piezocatalytic reaction rate (k value = 0.0746 min−1) was 4.63 times and 10.97 times higher than that of pure SrTiO3 and pure ZnO, respectively. Reactive species scavenger tests, electron paramagnetic resonance techniques, and bands gap analysis revealed that the enhanced activity can be attributed to the construction of an interfacial electric field in SrTiO3/ZnO heterojunctions and the modification of an internal piezoelectric polarized field. This allowed charge redistribution and transport across the SrTiO3/ZnO heterojunction interface, and facilitated the generation of hydroxyl radicals (HO•) through simultaneous hole oxidation and electron reduction. This study provides a comprehensive mechanistic understanding about piezoelectric heterojunctions in the catalytic redox reactions, and offers valuable insights for designing more effective piezoelectric heterojunctions for the degradation of pharmaceutical organic pollutants.