Theory predicts Cu-doped ZnO (ZnO:Cu) has p-conductivity; however, this has only been demonstrated in a small number of experimental and mechanistic studies. In this paper, ZnO:Cu films were grown insitu with varying Cu content, prepared using radiofrequency atomic source-assisted molecular-beam vapor deposition. The results indicate that ZnO:Cu films with dopant of Cu2+ only had n-type behavior. As the Cu content increased, Cu+ was the major dopant and the ZnO:Cu films had p-type behavior. However, excess Cu dopant resulted in the formation of second phases of Cu2O and Cu-Zn. The formation of a Cu-Zn phase increased the content of Zn vacancy, thus increasing hole concentration. Stronger alloy scattering decreased carrier mobility. Therefore, Cu+ dopant and Zn vacancy give ZnO:Cu films p-conductivity properties.