We propose negatively charged oxygen species at grain boundaries may be detrimental to the p-type behavior. After ultraviolet illumination to release oxygen species, the p-type behavior of moderately Na-doped ZnO films is strengthened in the subsequent several minutes. A robust p-type film with a hole mobility of 7.9 cm2/Vs, a hole concentration of 2.1 × 1017 cm−3, and a film resistivity of 3.8 Ωcm has been reproducibly achieved. Transformation from n-type to p-type conduction is observed for the lightly Na-doped ZnO after ultraviolet illumination. We believe that single crystalline p-type ZnO films are indispensable for ZnO light-emitting diodes.