CuO is an earth-abundant, nontoxic, and low band-gap material; hence it is an attractive candidate for application in solar cells. In this paper, a synthesis of CuO nanocrystals by a facile alcohothermal route is reported. The nanocrystals are dispersible in a solvent mixture of methanol and chloroform, thus enabling the processing of CuO by solution. A bilayer solar cell comprising of CuO nanocrystals and phenyl-C61-butyric acid methyl ester (PCBM) achieved a power conversion efficiency of 0.04%, indicating the potential of this material for light-harvesting applications.