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Aerobic oxidative desulfurization (AODS) promises to be a sustainable alternative technology for diesel desulfurization, which necessitates the efficient aerobic oxidation of thiophenic sulfides at mild conditions. Here we synthesize cerium phosphate (CePO4) nanowire-supported vanadium oxide (VOx) nanoclusters, controllably creating coordination-unsaturated V sites for boosting the AODS reaction. We propose that the electron transfer from a Ce species to a V site gives rise to the donor state and enhances its electron-donating capability for the activation of O2. We show that the catalyst possesses a higher specific activity than state-of-the-art vanadium oxide catalysts, activates reaction at 90 °C (5.17 mmol g–1 h–1), and achieves rapid conversion of various thiophenes under mild conditions. The catalyst demonstrates excellent durability in six cycles of reuse by maintaining an unchanged catalytic performance, a chemical structure, and a physical structure and is expected to act as a sustainable, efficient, and stable AODS catalyst. [ABSTRACT FROM AUTHOR]