Heterobimetallic aluminum copper and aluminum zinc clusters were prepared from the reaction of LAI(SeH)(2) [1; L = HC(CMeNAr)(2) and Ar = 2,6iPr(2)C(6)H(3)] with (MesCu)(4) and ZnEt2, respectively. The resulting clusters with the core structures of A(l2)Se(4)Cu(4) and Al2Se4Zn3 exhibit unique metal-organic frameworks. This is a novel pathway for the synthesis of aluminum copper and aluminum-zinc selenides. The products have been characterized by spectroscopic methods and single-crystal X-ray structural characterization.