Organosulfides have great significance and value in synthetic and biological chemistry. To establish a versatile and green methodology for C-S bond generation, we successfully developed a new aerobic cross-dehydrogenative coupling of C-H and S-H to synthesize aryl sulfides in water, utilizing CoPcS as the catalyst and O2 as the oxidant. This protocol shows great tolerance of a wide range of substrates. A large variety of organosulfur compounds were produced in modest to excellent yields.