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Using CBr4 as a mild oxidant, the direct C−H bond oxidation of N‐aryltetrahydroisoquinolines was achieved, giving a series of the corresponding iminium salts in high yields under metal‐ and photo‐free reaction conditions. This reaction is superior in high yields and good functional group tolerance, and the late‐stage derivatization showed that these iminium salts can readily be applied to the synthesis...