The synthesis, structure, and magnetic properties of a ligand-modified Mn-4 dicubane single-molecule magnet (SMM), [Mn-4(Bet)(4)(mdea)(2)(mdeaH)(2)] (BPh4)(4), are presented, where the cationic SMM units are significantly separated from neighboring molecules in the crystal lattice. There are no cocrystallized solvate molecules, making it an ideal candidate for single-crystal magnetization hysteresis and high-frequency electron paramagnetic resonance studies. Increased control over intermolecular interactions in such materials is a crucial factor in the future application of SMMs.