Two classes of Ni-Ln clusters [Ln4Ni3L3(OAc)6(NO3)3(OH)3] (Ln = Gd (1) and Tb (2)) and [Ln6Ni7L6(OAc)12(OH)6](OH)2 (Ln = Gd (3) and Dy (4)) were prepared using a specifically designed Schiff base ligand built around a flexible (CH2)2O(CH2)2O(CH2)2 chain. 1 and 2 exhibit cone-like structures, while 3 and 4 have nanosized sandwich architectures. The structures were studied by single-crystal X-ray diffraction and TEM, and magnetic properties were investigated.