High hole concentration Li-doped NiZnO thin films were grown by metal–organic chemical vapor deposition (MOCVD). The crystalline, optical, electrical, and morphological characteristics of the NiZnO films were studied as a function of lithium content. The resistance of the films decreased and the hole concentration greatly increased with increasing lithium content. However, the crystalline and optical properties were observed to degrade as the lithium content was increased. To relieve the degradation, a photo-assisted MOCVD method was used in order to restrict this degradation and this represents a new way to obtain stable high hole concentration NiZnO films.