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Coordination cages sustained by metal–ligand interactions feature polyhedral architectures and well-defined hollow structures, which have attracted significant attention in recent years due to a variety of structure-guided promising applications. Sulfonylcalix[4]arenes-based coordination cages, termed metal–organic supercontainers (MOSCs), that possess unique multi-pore architectures containing an <i>endo</i> cavity and multiple <i>exo</i> cavities, are emerging as a new family of coordination cages. The well-defined built-in multiple binding domains of MOSCs allow the efficient encapsulation of guest molecules, especially for drug delivery. Here, we critically discuss the design strategy, and, most importantly, the recent advances in research surrounding cavity-specified host–guest chemistry and biomedical applications of MOSCs.