In summary, 1 is structurally rather unusual and is a rareexample of 3d-metal clusters with O and N ligation, whichexhibits an interesting SMM behavior and highlights thepotential for creating improved SMMs by using CoIIions asmetal centers. Our results further support the idea thatjudiciously assembling “super-clusters” with anisotropicshapes from other [M4O4] cubanes as building blocks mayresult in magnetic relaxation effects at higher temperaturesthan that observed for 1 and allow us to probe the effects onSMM behavior of linking two or more clusters.