Engineering the band-edge of photocatalysts is one of the important strategies to adjust the photocatalytic performance. Herein, we successfully prepare Cu-Fe2O3/Ni-ZnO nanoplate photocatalysts and confirm by a series of materials characterization. The prepared Cu-Fe2O3/Ni-ZnO nanoplate exhibits the highest photodegradation performance of tetracycline among all the prepared samples. The experimental results demonstrate that introducing elements into Fe2O3/ZnO regulates the potentials of the conduction band and valence band, accelerating the recombination of Cu-Fe2O3 photogenerated electrons with Ni-ZnO holes. Furthermore, electron spin resonance (ESR) spectroscopy reveals that rapid production of reactive oxygen species (ROS) such as •O2 – and •OH can improve the photodegradation activity of Cu-Fe2O3/Ni-ZnO. This work reveals that engineering the band-edge of photocatalysts can be considered as an effective method to improve the photocatalytic activity.