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The introduction of enlarged and interconnected nanochannels into metal–organic frameworks (MOFs) overcome their micropore size restriction, enhances mass transportation, and improves the accessibility of anchored metal clusters. Herein, foamed Ce‐MOF single crystals (F‐Ce‐MOF‐SC‐x) designed from a multiscale co‐assembly is reported in the presence of a copolymer template and 1,3,5‐trimethylbenzene...