Introducing magnetic impurities into clusters of simplemetals can create localized states for higher angular momentum quantumnumbers (l = 2 or 3) that can breed magnetism analogous to that invirtual bound states in metallic hosts, offering a new recipe for magneticsuperatoms. In this work, we demonstrate that MnCan clusterscontaining 6−15 Ca atoms show a spin magnetic moment of 5.0 μBirrespective of the cluster size. Theoretical analysis reveals that the Mn dstates hybridize only partially with superatomic states and introduce extramajority and minority d states, largely localized at the Mn site, with alarge gap. Successive addition of Ca atoms introduces superatomic statesof varying angular momentum that are embedded in this gap, allowingcontrol over the stability of the motifs without altering the moment. Assemblies of such clusters can offer novel electronic features due to theformation of localized magnetic “quasibound states” in a confined nearlyfree electron gas.