Photochemical Nickel‐Catalyzed Hydrocyanation of Unactivated Alkenes Using Isonitriles ^†

Comprehensive Summary We report a practical, light‐driven nickel‐catalyzed hydrocyanation of alkenes using readily available isonitriles as cyanide surrogates. This method proceeds under mild conditions, tolerates a wide range of functional groups, and delivers linear alkyl nitriles with high efficiency and excellent regioselectivity. The protocol is broadly applicable, including to the late‐stage functionalization of complex, bioactive molecules derived from natural products and pharmaceuticals, providing a direct route to valuable nitrile‐containing building blocks and facilitating rapid access to drug‐like scaffolds.