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High-energy (>1.6 MeV) electrons create acceptors and donors in single-crystal ZnO. Greater damage is observed for irradiation in the [0001] direction (Zn face) than in the [0001̄] direction (O face). The major annealing stage occurs at about 300–325 °C, and is much sharper for defects produced by Zn-face irradiation, than for those resulting from O-face irradiation. The defects appear to have a chain character, rather than being simple, near-neighbor vacancy/interstitial Frenkel pairs. These experiments suggest that ZnO is significantly more “radiation hard” than Si, GaAs, or GaN, and should be useful for applications in high-irradiation environments, such as electronics in space satellites.