ZnO(0001) bulk crystals were implanted with 100 keV H2 + ions with various doses in the range of 5×1016 to 3×1017 cm-2. The ZnO crystals implanted up to a dose of 2.2×1017 cm-2 did not show any surface exfoliation, even after post-implantation annealing at temperatures up to 800°C for 1 h while those crystals implanted with a dose of 2.8×1017 cm-2 or higher exhibited exfoliated surfaces already in the as-implanted state. In a narrow dose window in between, controlled exfoliation could be obtained upon post-implantation annealing only. Cross-sectional transmission electron microscopy (XTEM) of the implanted ZnO samples showed that a large number of nanovoids were formed within the implantation-induced damage band. These nanovoids served as precursors for the formation of microcracks leading to the exfoliation of ZnO wafer surfaces. In addition to the nanovoids, elongated nanocolumns perpendicular to the ZnO wafer surfaces were also observed. These nanocolumns showed diameters of up to 10 nm and lengths of up to 500 nm. The nanocolumns were found in the ZnO wafer even well beyond the projected range of hydrogen ions.