The reaction of N-pyridylindolines with CO andethylene in the presence of Ru3(CO)12 results in directcarbonylation at a C−H bond δ to the pyridine sp2 nitrogen,which represents a new type of C−H/CO/olefin coupling. Thepresence of a pyridine ring as a directing group on thesubstrates is essential for the reaction to proceed. The choiceof N,N-dimethylacetamide (DMA) as the solvent is crucialfor the reaction to proceed efficiently.