Photocatalytic aerobic oxidation desulfurization (PAODS) is a promising and sustainable alternative to conventional, energy-intensive desulfurization techniques for petroleum products. However, its development is greatly plagued by the low capability in generating highly reactive oxygen species and sluggish kinetics of sulfide oxidation of reported photocatalysts. Here we report a class of MoO_x nanocluster decorated on ultrathin Mo-doped TiO₂ nanosheet (MoO_x/MoTiO) catalyst for efficiently facilitating the photocatalytic aerobic oxidation of sulfides. We demonstrate that MoO_x/MoTiO can not only promote the generation of highly reactive singlet oxygen (¹O₂) but also enhance the aerobic conversion of sulfides, which leads to a record dibenzothiophene oxidation activity of 3.90 mmol g⁻¹ h⁻¹. The multiple experimental characterizations and density functional theory calculations collectively reveal that the doped-Mo sites can interact with the photogenerated excitons, enabling directly energy transfer generation of ¹O₂ through a new exciton modulation mechanism, and the coordination unsaturated MoO_x clusters play the role of co-catalyst to enhance the separation of charge carriers, and effectively catalyze the reaction between sulfides and ¹O₂ to form sulfones.