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Superatoms are promising as new building block materials that can be designed by precise controlling of the constituent atoms. Stannaspherene (Sn122−) is a rigid cage‐like cluster with icosahedral symmetry, for which one‐atom encapsulation was theoretically expected and detected in the gas phase. Here, a single‐atom introduction method into stannaspherene using a dendrimer template with polyvinylpyrrolidone...