A formal C‐H carboxylation of unactivated arenes using CO2 in green solvents is described. The present strategy combines a sterically controlled Ir‐catalyzed C‐H borylation followed by a Cu‐catalyzed carboxylation of the in situ generated organoboronates. The reaction is highly regioselective for the C‐H carboxylation of 1,3‐disubstituted and 1,2,3‐trisubstituted benzenes, 1,2‐ or 1,4‐symmetrically substituted benzenes, fluorinated benzenes and different heterocycles. The developed methodology was applied to the late‐stage C‐H carboxylation of commercial drugs and ligands.

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