Whereas solar photovoltaic cells are promising for proper power production,their wide deployment is hampered by production costs, material availability and toxicity. One of these materials is CuO, which has great chemical stability as well as interesting physical properties, including a direct band gap, a high absorption coef cient, and p-type conductivity. These properties indicate CuO as an exciting semiconducting material to use an absorber layer in thin lms solar cells. For this speci c reason, this paper focuses on the synthesis of undoped and Ni-doped CuO thin lms by spray pyroly- sis process. Several techniques such as; X-ray diffraction (XRD), Raman spectroscopy, Scanning Electron Microscopy (SEM), Energy dispersive X-ray (EDX) and UV-Visible spectroscopy have been employed to characterize the synthesized samples. The XRD analysis indicated the formation of polycrystalline CuO thin lms and the average crystallite size was decreased from 35 to 20 nm for the samples with x = 0 to 8 at%, respectively. Furthermore, Raman spectroscopy also con rms the single-phase formation of CuO lms. The SEM images demonstrated that the incorporation of Ni in the CuO matrix improved the lms surface. The EDX analysis and the elemental mapping belay the homogeneous distribution of the elements. Moreover, UV-Visible spectroscopy has shown a signi cant expansion in optical energy band gap from 1.45 to 1.53 eV with an increase of Ni concentration. On the other hand, to investigate the impact of Ni-doped CuO on nanos- tructure Ni:CuO/ ZnO-NRs heterojunction solar cell performance, SCAPS-1D software is used. It has been found that, 8% Ni:CuO layer has been revealed as better for nanostructured solar cells. The results of this contribution will provide some vital guidelines for fabricating higher-ef ciency solar cells.