Desulfurization of organosulfur compounds is a highly important reaction because of its relevance to the hydrodesulfurization (HDS) process of fossil fuels. A reaction system involving Co(BF4)(2)center dot 6H(2)O and the dinucleating ligands HBPMP or HPhBIMP has been developed that could desulfurize a large number of thiophenes, sulfides, and thiols to generate the complexes [Co-2 (BPMP) (mu(2)-SH) (MeCN) (BF4)(2) (1a), [Co-2 (BPMP) (SH)(2)] (BF4) (1b), and [Co-2 (PhBIMP) (mu(2)-SH) (X)] (BF4)(2) [X = DMF (2a), MeCN (2c)], while the substrates are mostly converted to the corresponding alcohols/phenols. This convenient desulfurization process has been demonstrated for 25 substrates in 6 different solvents at room temperature.