High quality copper oxide thin films were prepared by nebulizer spray pyrolysis technique using different concentrations of copper precursor solution. Concentration-dependent structural, morphological, optical, and electrical properties of the prepared films are discussed. X-ray diffraction studies done for the samples confirmed that the deposited films are in Cu 2 O phase with polycrystalline cubic structure. Atomic force microscopy analysis revealed that all the films are composed of nano sheet shaped grains covering the substrate surface. Optical studies done on the samples showed band gap values 2.42, 2.31, and 2.02 eV for the solution concentration 0.01, 0.05, and 0.1 M, respectively. Photoluminescence spectral analysis showed the emission band at 620 nm confirming the formation of cuprous oxide. Electrical analysis of the films showed p-type conductivity with a low resistivity 2.19 × 10 2 Ω.cm and high carrier concentration 16.76 × 10 15 cm −3 for the molar concentration 0.1 M. In this work, Cu 2 O/ZnO heterojunctions were also prepared, and solar cell properties were studied; they were found to show increased open circuit voltage and short circuit current for higher copper concentration.