Developing sustainable and atom-economical hydrogen transfer routes for constructing pharmacologically valuable quinoline scaffolds from abundant alcohol feedstocks remains a significant challenge. Herein, a tailored pyridinic-nitrogen-coordinated cobalt (Co) single-atom catalyst (Co-N/C-U) is showcased, enabling the efficient synthesis of quinoline derivatives from inexpensive and readily available 2-nitrobenzyl alcohol and various secondary or primary alcohols via a cascade hydrogen transfer p