A bifunctional ligand, 2,2'-bipyridine-4,4'-dicarboxylic acid (Hbpdc), has been used in the investigation of constructing bimetallic uranyl organic frameworks (UOFs). Seven novel uranyl-transition metal bimetallic coordination polymers, [(UO)Zn(bpdc)] (1), [Cd(UO)(bpdc)(HO)·2HO] (2), [Cu(UO)(bpdc)(SO)(HO)·2HO] (3), [CuCl(UO)(bpdc)(Hbpdc)(HO)·HO] (4), [Cu(UO)(bpdc)(HO)] (5), [Co(UO)(bpdc)] (6), and [Co(UO)(bpdc)(Hbpdc)(HO)] (7), have been successfully constructed through the assembly of various transition-metal salts, uranyl ions, and Hbpdc ligands under hydrothermal conditions. UOFs 1, 5, 6, and 7 adopt three-dimensional (3D) frameworks with different architectures; UOFs 2 and 3 exhibit two-dimensional (2D) wavelike and stairlike layers, respectively, while UOF 4 is a one-dimensional (1D) chain assembly. These UOFs include a wide range of dimensionalities (1D-3D), interpenetrated frameworks, and cation-cation interaction species, suggesting that anion-dependent structure regulation based on the metalloligand [M(bpdc) ] motifs, the coordination modes of the metal centers and bpdc ligands, along with the reaction temperature, has a remarkable influence on the formation of bimetallic UOFs, which could be a representative system for the structural modulation of UOFs with various dimensionalities and structures. Furthermore, the thermal stability and luminescent properties of compounds 1, 3, and 6 are also investigated.