Generating enantiomerically enriched nitriles in which the cyano group is bound to an all- carbon quaternary stereocenter (eg 1) is an important challenge in synthetic organic chemistry and is owed in part to the biological activity of such compounds.[1] We have recently turned our attention to the development of catalytic asymmetric methods that address this challenge [2, 3] by focusing on reactions of nitrile anions.[4] Such species are ...