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Oxynitrides are considered as new potential candidates for photocatalysis due to their lower bandgap compared with traditional oxide photocatalysts. However, the formation of native nitrogen monovacancies during the synthesis of oxynitrides reduces their photocatalytic activity due to the vacancy-induced electron/hole recombination. This study shows that a transition from the native nitrogen monovacancies to the nitrogen-based vacancy complexes in a GaN–ZnO oxynitride not only diminishes the recombination but also enhances the photocatalytic hydrogen production. Here, the vacancy complexes are introduced by mechanical straining via the high-pressure torsion (HPT) method and it is shown that the vacancy complexes reduce the bandgap and increase the over-potential for hydrogen production on the conduction band. The current results introduce a simple but effective approach to turn the nitrogen …