The formation of highly resistive films of single-crystal ZnO as a result of irradiation with MeV Li, O, and Si ions is demonstrated. Results show that the ion doses necessary for electrical isolation close-to-inversely depend on the number of ion-beam-generated atomic displacements. Results show that an increase in the dose of 2 MeV O ions (up to ∼ 2 orders of magnitude above the threshold isolation dose) and irradiation temperature (up to 350 °C) has a relatively minor effect on the thermal stability of electrical isolation, which is limited to temperatures of ∼ 300 — 400 °C. For the case of multiple-energy implantation with keV Cr, Fe, or Ni ions, the evolution of sheet resistance with annealing temperature is consistent with defect-induced isolation, with a relatively minor effect of Cr, Fe, or Ni impurities on the thermal stability of isolation. Based on these results, the mechanism for electrical isolation in ZnO by ion bombardment is discussed.