Two novel 3D heterometallic coordination polymers, Ln(4)(mu(3)-OH)(2)Cu6I5(IN)(8)(OAc)(3) (Ln = Nd (1), Pr (2); HIN = isonicotinic acid, HOAc = acetic acid), have been synthesized under hydrothermal conditions and characterized by elemental, infrared, and thermogravimetric analyses and single-crystal X-ray diffraction. Both compounds are isostructural and crystallize in the monoclinic system, space group P2(1)/c. Both polymers are constructed from 2D lanthanide-cluster polymers based on the {Ln(16)} wheel-cluster and 1D copper-cluster polymers based on the {Cu6I5} cluster, which represent the first examples of 3D coordination frameworks created by using a combination of two different types of metal-cluster polymer units, namely, a high-nuclearity lanthanide-cluster polymer and a transition-metal-cluster polymer.