Heterogeneous catalysts show superior separable and recyclable property in comparison with homogeneous catalysts. However, the conventional synthetic method faces the problem of uneven distribution of active sites. Here, a facile dissolution-regrowth strategy was developed to prepare hollow mesoporous silica nanospheres supported cobalt molybdate (CoMoO₄/HMS) under mild conditions, simultaneously, CoMoO₄ was obtained in situ. The homogenous dispersion of the active species made the catalyst manifest an outstanding desulfurization efficiency in aerobic oxidative desulfurization compared with the supported single-metal oxides catalysts or supported CoMoO₄ catalyst prepared by wet impregnation. The removal efficiency of three sulfur-containing substances, such as dibenzothiophene, 4-methyldibenzothiophene and 4,6-dimethyldibenzothiophene, could reach 100% by 5 h with molecular oxygen as an oxidant. Besides, the sulfur removal of DBT almost did not reduce after at least 8 cycles under the optimal reaction conditions. Through electron spin resonance spectroscopy and radical quenching experiments, O₂⁻ was determined as the main active oxygen species for sulfur oxidation. This dissolution-regrowth strategy can be used to prepare a series of supported multi-metal oxides for various applications.