Radical‐mediated Hydrogen Atom Abstraction of Csp3−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
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