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The supramolecular self‐assembly of the outer surface of cucurbit[n]uril is one of the main areas of focus in cucurbit[n]uril chemistry. The crystal structure is determined by single‐crystal X‐ray diffraction and characterized. This work focuses on the supramolecular self‐assembly between CyP5Q[5], FeCl2, FeCl3 and CyP6Q[6] and HClO4 through the interaction of the outer surface.