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Bismuth telluride alloys favor the applications of low‐grade waste heat recovery if their figure‐of‐merits are improved within the larger temperature range from 300 to 523 K. Herein, this work reports a synergistic optimization for Bi0.5Sb1.5Te3 (BST) by incorporating the copper(II) phthalocyanine (CuPc), which is preferentially distributed at the grain boundary of BST after the spark plasma sintering...