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Second harmonic generation (SHG) and X-ray diffraction rocking curves of high-quality ZnO single crystals implanted by different ions (He, Cu, and Zn) were investigated. Interestingly, it was found that both He- and Zn-implanted samples show a convinced increment in SHG efficiency while the Cu-implanted one does not. X-ray diffraction rocking curves of the samples show satellite structures, and the simulations firmly reveal the formation of quasi-interfaces inside He- and Zn-implanted crystals. These quasi-interfaces lead to SHG improvement in the two samples. Polarization dependence of SHG of the samples on the excitation light also evidences this conclusion.