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The C(sp3)−H bond decyanative arylations of diverse symmetrical and unsymmetrical BIMs have been successfully accomplished. Aromatic nitriles were utilized as components in the presence of thiobenzoic acid (TBA) under visible‐light irradiation. These redox‐neutral protocols provide a highly efficient and practical strategy for the synthesis of a broad range of bis(indolyl)‐substituted and mono(indolyl)‐substituted...