Dedicated to Professor Hansgeorg Schnöckel on the occasion of his 65th birthday.The first evidence of single molecule magnet (SMM) behavior was discovered in the mixed-valence compounds [Mn [1] In the quest to synthesize SMMs that show hysteresis at higher temperatures, it has been recognized that large ground-state spins and a uniaxial anisotropy (large negative D and small E considering the following Hamiltonian anisotropy term:It is thus of interest to discover how to obtain the largest-spin ground state possible for a given size of aggregate. As well as having four unpaired electrons in its high-spin state, the Mn III ion is particularly useful for introducing large anisotropies through the presence of Jahn-Teller distortions in this configuration and has been the most thoroughly studied candidate for synthesizing new SMMs. Amongst the large number of aggregates containing manganese(III) in the literature, a Mn 25 cluster has been reported as having a ground spin state of 51/2.[4] Herein we report on the realization of the maximum-spin ground state of 83/2 for the aggregate [Mn

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