Abstract: High-sulfur bauxite is an important aluminum mineral resource in China. However, the excessive sulfur content in bauxite significantly hinders the normal production of aluminum oxide. Therefore, developing an effective desulfurization process for high-sulfur bauxite is of great significance for ensuring a stable aluminum supply in China. A high-sulfur bauxite sample from Guangxi contains 4.72% sulfur, with pyrite as the primary sulfur-bearing mineral, closely intergrown with diaspore and kaolinite. The fine and uneven distribution of these minerals increases the complexity of the desulfurization process. In this study, flotation was employed for desulfurization, and the effects of grinding fineness, regulators, and collector structure on flotation performance were systematically investigated to optimize the flotation parameters. The selective adsorption behavior of isobutyl xanthate on sulfur minerals was also explored. Using a combination of sodium carbonate and copper sulfate, and isobutyl xanthate as the collector, a flotation flowsheet consisting of one roughing, two cleanings, and two scavenging stages was established. Closed-circuit tests yielded a high-quality bauxite concentrate with a recovery of 89.93% and a sulfur content of 0.44%, alongside a sulfur concentrate with a sulfur grade of 42.95%. These results demonstrate the efficient removal and comprehensive recovery of sulfur from high-sulfur bauxite, providing technical guidance for the industrial development of this ore type.