These results, alongside those we and others have already reported in the chemistry of p-t Bucalix [4]arene and 2,2'-bis-p-t Bu-calix [4]arene, suggest that the Mn III L metalloligand can be employed as a structure-directing unit capable of encapsulating additional TM (and LnM) moieties in its core. The ability to construct families of structurally analogous species, but whose oxidation state distribution, or metal identity, differs allows for more detailed investigation of the magneto-structural relationship. This ability underpins the design of magnetic molecules whose properties can be tuned toward a specific application. It also has wider design implications for scientists interested in molecules that can robustly cycle through multiple oxidation levels in, for example, bioinorganic chemistry and catalysis.