We report the realization of the p-type conductivity and the enhancement of the photoluminescence (PL) intensity in undoped ZnO films treated with high-energy (1 MeV) electron-beam irradiation (HEEBI), suggesting that the HEEBI process is compatible with a low-temperature requirement for the fabrication of transparent thin film transistors with good efficiency on a plastic substrate. The p-type conductivity of the films was revealed by the Hall, x-ray photoelectron spectroscopy, and PL measurements after being electron-irradiated in air at room temperature. The major acceptor-like defects were determined to be oxygen interstitial and zinc vacancy. A model was proposed in terms of O as well as Zn diffusion to explain the observed results. It was also observed that HEEBI treatment has little influence on the optical transmittance of ZnO films, whereas HEEBI treatment shifts the optical band gap toward the lower energy region from 3.29 to 3.28 eV.