A nitrogen-doped carbon supported nanocobalt catalyst was developed and successfully applied for the hydrogentransfer coupling of quinolinium salts and tetrahydroquinoline compounds. The selective coupling of the C6 sites of tetrahydroquinolines (THQs) with the α sites of quinoline salts generated a series of 2-substituted N-alkyl-tetrahydroquinolines. This catalytic conversion method, which can be employed to synthesize various functionalized tetrahydroquinolines, has several advantages that include excellent hydrogen transfer selectivity, a reusable and inexpensive catalyst, and environmental friendliness. Letter pubs.acs.org/OrgLett