Four novel U(VI) containing coordination polymers, UO2(C7H10O4) (1), UO2(C8H12O4) (2), UO2(C9H14O4) (3), and UO2(C10H16O4) (4), were synthesized from UO2(NO3)(2)center dot 6H(2)O and aliphatic dicarboxylic acids (pimelic, suberic, azelaic, and sebacic acids, respectively) using hydrothermal techniques and were characterized by single-crystal diffraction. Compounds 1 and 4 consist of (UO2)(2)O-8 dimers connected by the acid molecules to form layers, whereas 2 and 3 are constructed of chains of hexagonal bipyramids connected to form layers. These materials complete the series of aliphatic uranyl carboxylates to C-10 (sebacic acid) and may be considered to be carboxylate "end-members" of a series of dipyridyl/carboxylate structures described in part II of this investigation (following in this issue).