A nickel-catalyzed intermolecular arylcyanation of 8-aminoquinolinyl β,γ-unsaturated amides is reported. The three-component reaction directly afforded diverse β-cyano γ-aryl amides with exclusive chemo- and regioselectivity. The synthetic practicality of this approach is further demonstrated through multigram scale reaction, expanded transformations of the nitrile product, late-stage modification of complex molecules, and direct drug synthesis.