Morphological modulation of heterogeneous catalysts has been shown to be a useful strategy for adjusting the concentration or intrinsic activity of active sites and their catalytic activity in catalysis. Herein, a hierarchical porous TS-1-supported cobalt molybdate catalyst (CoMoO4/TS-1-DR) was obtained through a facile dissolution-regrowth strategy. In an oxidative desulfurization reaction using O2 as the oxidant, the as-prepared catalyst demonstrated exceptional performance compared to the supported catalyst prepared via the impregnation method due to the bimodal pore architecture presented. Moreover, in situ CoMoO4 synthesis lowers active site leaching, thus showing better reaction stability. After 7 recycles, the removal rate of DBT still remained at 88.8%. This work offers a generic in situ encapsulation strategy for designing hierarchical porous zeolite catalysts and the synthesis of loaded metal oxides.