Dual Nickel/Photoredox‐Catalyzed Asymmetric Carbamoylation of Benzylic C(sp3)−H Bonds

Abstract Radical‐mediated Hydrogen Atom Abstraction of Csp 3 −H bonds has become a powerful tool for the asymmetric functionalization of organic feedstocks. Here, we present an asymmetric synthesis of α ‐aryl amides via carbamoylation of alkylarenes with isocyanates as electrophiles. The synergistic combination of a photoredox and a chiral nickel‐catalyst, enables the use of readily available and neutral reagents under mild reaction conditions and provides straightforward access to pharmacologically relevant motifs in enantiomerically pure form.