Three uranyl carboxylates, namely, (UO2)(L-1)(H2O)(0.5) (1), [(UO2)(L-2)(H2O)]center dot 2H(2)O (2), and [(UO2)(L-2)(H2O)]center dot(CH3CN) (3), were synthesized hydrothermally from 2',3',5',6'-tetramethyl-(1,1':4',1 ''-terphenyl)-4,4 ''-dicarboxylic acid (H2L1) and 2',5'-dimethyl-(1,1':4',1 ''-terphenyl)-3,3 ''-dicarboxylic acid (H2L2), which are all steric carboxylic acid ligands but vary with the carboxylic acid group position and methyl group number. It is found that compound 1 displays a three-dimensional 8-fold-interpenetrated net with channels running along the c direction. Compounds 2 and 3 are isostructural, and all display two-dimensional-layered crystal structures but contain different guest molecules. The photophysical measurements reveal that compounds 1 and 2, which contain disordered water molecules, are luminescence-quenched, whereas compound 3 containing acetonitrile molecules is luminescent.