Single-molecule magnets (SMMs) have attracted considerable interest in recent times.[1] Although molecular, these species display superparamagnetic properties normally seen in mesoscale magnetic particles and thus can function as magnetizable entities below their blocking temperature. As a consequence, they represent the ultimate limit of miniaturization for data-storage domains in magnetic media.[1] Quantum tunneling of magnetization (QTM) effects [2] have led to the proposal that SMMs could be exploited as qubits in quantum computing.[3] The existence of SMM behavior was first noted ten years ago in the complex [Mn 12 O 12 (O 2 CMe) 16 (H 2 O) 4 ] (S = 10, D = À0.50 cm À1 = À0.72 K), [4] which represents the most extensively studied SMM.[1] Another compound that has been investigated for its SMM behavior is [{Fe 8 O 2 (OH) 12 (tacn) 6 }Br 7 ·H 2 O]Br·8 H 2 O (tacn = 1,4,7-triaza-