Solar cells are produced by atomic layer deposition (ALD) of n‐type amorphous zinc‐tin‐oxide buffer layers on electrochemically deposited p‐type cuprous oxide, Cu2O, absorber layers. The diethylzinc precursor in the ALD process reduces Cu2+‐related defects at the heterojunction interface, improving the solar‐cell open‐circuit voltage. An NREL‐certified power conversion efficiency of 2.85% is reported.