A new low symmetry octanuclear cyano-based {Fe(III)(4)Ni(II)(4)} single-molecule magnet (SMM) is described. This SMM exhibits the highest energy barrier (Delta/k(B) approximately 33 K) for magnetization reversal seen for any first-row cyanide-based complex. The importance of anisotropy axes alignment and their impact on SMM properties are illustrated when cubic {Fe(III)(4)Ni(II)(4)} boxes are compared to octanuclear complexes of lower overall symmetry.