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O2•-, as well as photogenerated holes, have been proven to be the dominant active species for the photodegradation of phenol. 25CH4-ZnGaNO, with the lowest density of bulk defects and the highest density of surface VO, exhibited the best photoactivity under visible-light irradiation for the photodegradation of Rhodamine B and phenol. The obtained surface-VO-rich (GaN)0.5(ZnO)0.5 particles can be applied as a high-performance visible-light-driven photocatalyst in the photodegradation of organic pollutants.Volatile methyl sil