Using ZnO seed layers, an efficient approach for enhancing the heterointerface quality of electrodeposited ZnO–Cu₂O solar cells is devised. We introduce a sputtered ZnO seed layer followed by the sequential electrodeposition of ZnO and Cu₂O films. The seed layer is employed to control the growth and crystallinity and to augment the surface area of the electrodeposited ZnO films, thereby tuning the quality of the ZnO–Cu₂O heterointerface. Additionally, the seed layer also assists in forming high quality ZnO films, with no pin-holes, in a high pH electrolyte solution. X-ray electron diffraction patterns, scanning electron and atomic force microscopy images, as well as photovoltaic measurements, clearly demonstrate that the incorporation of certain seed layers results in the alteration of the heterointerface quality, a change in the heterojunction area and the crystallinity of the films near the junction, which influence the current density of photovoltaic devices.