This Article provides a simple new protocol for the preparation of valuable aryl-alkyl linkages that were, in many cases, either difficult or impossible to directly access. Multiple enabling applications are disclosed that can dramatically reduce step-count to such structures. The reaction can be reliably scaled in both flow and batch settings. Finally, CV studies, titration experiments, control studies with Ni(0) and Ni(II)-complexes, and ligand optimization data offer insights into the role of the BINAP/pyridine-system in enabling the challenge formation of all-carbon quaternary centers with high isomeric ratio. Given the immediate uptake of this method by the industrial co-authors of this study, broad utility of this electrochemical cross coupling is anticipated.