Soft d 10 metal ions (M), such as Au I and Ag I , show metallophilicity and form M···M interactions despite their electrostatic repulsion. [1] Although there are many examples of onedimensional arrays of these metal ions both in solution and in the solid state, [2] three-dimensionally controlled ionic clusters of these metals have seldom been synthesized. [3] We recently prepared a [3 3] Au I 9 cluster, [4] which consists of three layers of planar Au I 3 complex 2 a, in the confined cavity of selfassembled cage 1 a (Figure 1). Here, we report that trinuclear Au I 3 complex 2 b takes up silver ions to form an unprecedented triple-decker ion cluster (Au 3 -Ag-Au 3 -Ag-Au 3 ) in the cage. There is only one example of a double-decker sandwich cluster, Au 3 -Ag-Au 3 , prepared by the co-crystallization of a Au I trinuclear complex with a silver ion. [5] However, this structure is only observable in the solid state, and higher or infinite multi-decker clusters have never been [*] T.