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The utility of microporous coordination polymers (MCPs) for the adsorption of large organosulfur compounds (benzothiophene, dibenzothiophene, 4,6-dimethyldibenzothiophene) found in fuels is demonstrated. Large capacities are obtained at both low and high sulfur concentrations. For 4,6-dimethyldibenzothiophene, the compound most difficult to remove using current industrial techniques, a capacity of 41 g S/kg MCP at 1500 ppmw S is achieved by UMCM-150. It was determined that the size/shape of the pores in the MCP, rather than the surface area or pore volume, is the most important factor controlling adsorption capacity.