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Commercialization of high energy density Lithium‐Sulfur (Li‐S) batteries is impeded by challenges such as polysulfide shuttling, sluggish reaction kinetics, and limited Li+ transport. Herein, a jigsaw‐inspired catalyst design strategy that involves in situ assembly of coherent nano‐heterocrystal ensembles (CNEs) to stabilize high‐activity crystal facets, enhance electron delocalization, and reduce...