Precisely controlling the product selectivity from the complex reaction is always an attractive topic in the catalysis field. In this paper, the Ru/strong base junction formed by the redox strategy was demonstrated as an efficient catalyst to switch the selectivity in aerobic oxidation of benzylamines. The zirconia-supported ruthenium (Ru-ZrO 2 ) catalyst could catalyze benzylamine oxidation coupling to imines; however, the potassium oxide strong base modified zirconia-supported ruthenium (Ru-K-ZrO 2 ) catalyst could catalyze benzylamine oxidation dehydrogenation to nitriles. Insight into the mechanism showed that the base modified catalyst had excellent dehydrogenation ability which was assisted by the C-H bond activation and changed the reaction pathway. The strong base modified strategy may provide a new approach for controlling the performance of heterogeneous catalysts and product selectivity.