Two discrete nitrate-bridged novel "pseudo-double-propeller"-shaped hexanuclear Cu/Ln dusters of the formula [Cu(4)Ln(2)L(4)L(4)'(NO3)(2)(OH2)(2)]center dot 3NO(3)center dot 4H(2)O [Ln = Dy, Gd; LH = o-vanilin; L'H = 2-(hydroxyethyl)pyridine] were synthesized and characterized. Single-crystal X-ray diffraction studies revealed the trimeric half-propeller-type Cu-2/Ln core connected to other opposite-handed similar trimers by a bridging nitrate ligand. The Dy analogue, [Cu4Dy2L4L4'(NO3)(2)(OH2)(2)]center dot 3NO(3)center dot 4H(2)O, shows frequency-dependent out-of-phase alternating-current magnetic susceptibility, which indicates that this novel discrete [Cu4Dy2] heterometallic cluster may exhibit single-molecule-magnet behavior.