The synthesis and structural characterization of the compounds K[(UO2)(2)(UO4)(OH)(NO3)(2)]H2O (1) and Ba[(UO2)(4)(UO4)(2)(OH)(2)-(NO3)(4)]H2O (2) have revealed that each contains sheets that are based upon the beta-U3O8-type topology and that these sheets are linked through low-valence interlayer cations. Consistent with other uranium(VI) compounds that have topologically identical sheets, one of the uranium(VI) sites exhibits a highly unusual (UO4)(2-) tetraoxido core that is further coordinated by two bidentate (NO3)(-) groups.