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We report a direct azidation of benzylic C(sp3)−H bonds via an electrochemical process, which use cheap and durable graphite plates as electrodes, without any external oxidants or metal catalysts. This protocol is a novel, green and environmentally benign synthetic strategy to achieve azidation of C(sp3)−H in benzylic group. More importantly, these azidation products are suitable for late‐stage functionalization to afford diversified triazole and tetrazole derivatives. [ABSTRACT FROM AUTHOR]