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In this study, we investigated the interaction of a fully substituted cyclopentano cucurbit[6]uril (CyP6Q[6]) with alkaline earth cations (AE2+) and corresponding supramolecular assemblies in the presence of tetrachloridozincate anions ([Zn(H2O)Cl3]− or [ZnCl4]2−). Single‐crystal X‐ray diffraction analysis revealed that the CyP6Q[6]−Mg2+−ZnCl2−HCl interaction system yielded an adduct of [Mg(H2O)6]2+ with CyP6Q[6]. The CyP6Q[6]−Ca2+, Sr2+ and Ba2+−ZnCl2−HCl interaction systems yielded linear AE2+/CyP6Q[6]/AE2+‐type coordination polymers that filled the cells in the [ZnCl4]2−‐based honeycomb‐like framework. Unlike unsubstituted Q[n] systems in which [ZnCl4]2− anions surround Q[n] molecules via outer surface interaction of Q[n], electrostatic interactions between [ZnCl4]2− anions and the coordinated AE2+ cations results in the formation of [ZnCl4]2−‐based honeycomb‐like frameworks.

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