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We observed an unusual reversible aggregation process showing stimuli-responsive structural dynamics and optical changes attributed to the formation of a sandwich-like Au3-Ag-Au3 cluster, which can be synthesized through both solution and mechanochemical methods.1 Unlike many other heteronuclear gold-silver clusters, the affinity of two cyclic Au3 complexes2 and a AgⅠ ion is solely bound by ligand unsupported Au-Ag bonding.