A palladium-catalyzed highly enantioselective allylic alkylation of pyrroles and 4,7-dihydroindoles has been successfully developed with the use of chiral alkene-phosphine hybrid ligands to furnish the desired products in high yields with excellent ee鈥檚. It is noteworthy that alkene鈥損hosphine ligands are much more effective than some other types of chiral ligands in this catalytic system.