A single-component Co(-I) catalyst, [(PPh<sub>3</sub>)<sub>3</sub>Co(N<sub>2</sub>)]Li(THF)<sub>3</sub>, has been developed for olefin hydroarylations with (<i>N</i>-aryl)aryl imine substrates. More than 40 examples were examined under mild reaction conditions to afford the desired alkyl-arene product in good to excellent yields. Catalysis occurs in a regioselective manner to afford exclusively branched products with styrene-derived substrates or linear products for aliphatic olefins. Electron-withdrawing functional groups (e.g., -F, -CF<sub>3</sub>, and -CO<sub>2</sub>Me) were tolerated under the reaction conditions.
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