The development of simple and highly effective desulfurization technology is attracting more and more interest in both industrial and academic fields. Here, a new family of precursors was prepared based on hyper-cross-linked asphalt and coal tar building blocks. Thanks to the preintroduced porous structure, the precursors were converted into carbons with high surface area and large micropore volume via a uniform carbonization process. The synergistic effects of high surface area, abundant microporous structure, and the introduced polar functional groups endow the carbon materials with high desulfurization performance. The results of repeated experiments show that the adsorption capacities of five carbonized samples are higher than 40 mg S g-1, and the theoretical maximum adsorption capacity reaches 44.7 mg S g-1. Particularly, the adsorption equilibrium of all the carbonized samples can be reached in 5 min. Moreover, the recycle adsorption performance was also studied. Toluene exhibits the best elution effect among three eluents (iso-octane, para-xylene, and toluene) and the adsorption capacity remains 89% of the initial adsorption capacity after two adsorption-desorption cycles. It is believed that both innocent treatment of byproducts from petroleum industry and their high-value application for deep desulfurization in liquid hydrocarbon fuels benefit environmental protection and sustainable development.