Syntheses of substituted anilines primarily rely on palladium‐catalyzed coupling chemistry with prefunctionalized aryl electrophiles. While oxidative aminations have emerged as powerful alternatives, they largely produce undesired metal‐containing by‐products in stoichiometric quantities. In contrast, described herein is the unprecedented electrochemical C−H amination by cobalt‐catalyzed C−H activation. The environmentally benign electrocatalysis avoids stoichiometric metal oxidants, can be conducted under ambient air, and employs a biomass‐derived, renewable solvent for sustainable aminations in an atom‐ and step‐economical manner with H2 as the sole byproduct. Zapping N: Electrochemical C−H aminations were realized in a biomass‐derived renewable solvent under mild reaction conditions. The method exploits electricity as a sustainable oxidant and H2 is the sole byproduct