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The combustion of fuel with high sulfur concentrations produces a large number of sulfur oxides (SO_x), which have a range of negative effects on human health and life. The preparation of catalysts with excellent performance in the oxidative desulfurization (ODS) process is highly effective for reducing SO_x production. In this paper, cross-linked polyvinylimidazole (VE) was successfully created using a simple ontology aggregation method, after which a catalyst of polyvinylimidazolyl heteropolyacid clusters (VE-HPA) was prepared by adding heteropolyacid clusters. Polyvinylimidazolyl-phosphotungstic acid (VE-HPW) showed an outstanding desulfurization performance, and the desulfurization efficiency reached 99.68% in 60 min at 50 °C with H₂O₂ as an oxidant. Additionally, the catalyst exhibited recyclability nine consecutive times and remained stable, with a removal rate of 98.60%. The reaction mechanism was eventually proposed with the assistance of the free radical capture experiment and GC-MS analysis.