With the increasing need for high-value utilization of diesel components, catalytic oxidative desulfurization (ODS) emerges as an efficient non-hydrogenation approach to desulfurization and utilization of aromatic sulfides. Although TiO2 is a promising candidate for ODS, the catalytic activity is limited. Herein, with the heterojunction interface formation, a series of TiO2/three-dimensional porous carbon nitride catalysts (Ti/3D g-C3N4) has been developed for ODS. Notably, the successful construction of the type II heterojunction between TiO2 and 3D g-C3N4 is confirmed through systematic characterizations. The bandgap is narrowed in the hybrid materials, accelerating the electron transfer from the N to the Ti center, conducive to the activation of hydrogen peroxide in the radical pathway. Also, the emergence of micro-mesoporous pores in 3D g-C3N4 enhances the adsorption mass transfer of aromatic sulfides. The synergistic effect between heterostructures and extended mesopores generates superoxide radicals, attaining >99% adsorption-promoted catalytic oxidation reactivity of aromatic sulfides. The work develops bifunctional heterogeneous materials of efficient adsorption-promoted catalytic oxidation, expanding the development for the high-value utilization of sulfides in diesel fuel.