Two neutral, dizwitterionic dicarboxylates, N,N,Nʹ,Nʹ-tetramethylethane-1,2-diammonioacetate (L1) and biphenyl-4,4ʹ-diyl-bis(4-carboxylatopyridiniomethylene) (L2), have been used as ligands in syntheses of uranyl ion complexes which exemplify the effect of different reaction conditions. [UO2(L1)Cl2]·H2O (1) has been crystallized at room temperature and is a simple monoperiodic coordination polymer. In contrast, [(UO2)4(O)2(OH)2(C2O4)(L1)2]·4H2O (2), obtained under solvo-hydrothermal conditions, contains a tetranuclear, bis(µ3-oxido)-bridged cluster resulting from uranyl hydrolysis, and additional oxalate coligands most likely due to oxidative degradation of L1, and it crystallizes as a diperiodic coordination polymer with tetranuclear nodes and the sql topology. The same arrangement is found in [(UO2)4(O)2(OH)2(L2)3](I3)2·6H2O (3), also synthesized under solvo-hydrothermal conditions, but here the more oxidation-resistant ligand does not generate oxalate, and replacement of the latter by neutral L2 bridges makes this complex cationic. The very large cells of the network in 3 (~ 22 Å × 39 Å) accommodate the triiodide anions formed in situ.