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Metal–organic rotaxane frameworks (MORFs) attracted much attention in the past years for construction of intelligent functional materials. Herein, a one‐pot synthesis is reported of a three‐dimensional (3D) cucurbit[7]uril (Q[7])‐based MORF under hydrothermal conditions, namely Q[7]‐MORF‐1, formed by encapsulating the anionic benzoate moieties of the tricarboxylate ligand into the cavity of Q[7]....