A one-pot three-component route for the direct introduction of dithiocarbamates into indoles using a C-H sulfenylation strategy mediated by molecular iodine is disclosed. Various indole derivatives including 1-methylindole, 2-methylindole, 3-methylindole, and 5-substituted indoles were applied successfully in this protocol to afford diverse indole-dithiocarbamates containing the dithiocarbamate group on the position two or three in good to high yields. The reactions do not require transition metals or disulfiram but use an environmentally benign solvent and simple commercially available starting materials.