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Yingze Song and coworkers decipher the plasma‐triggered defect micro‐environment of graphene for highly efficient Li–S redox reactions. The defective graphene, especially the divacancies, effectively optimize the Li–S chemistry by selectively decelerating the generation of high‐order polysulfides and passingly promoting the conversion to Li2S product, shedding frontier light on practical Li–S batteries by designing specific defect‐type carbon structures. image