Nine new templated uranyl sulfates and selenates, [(H9O4)(2)(H2O)][(UO2)(2)(SO4)(3) (H2O)(2)] (H9US), [(C5H7NO)(2) (H2O)][(UO2)(2)(SO4)(3)(H2O)(2)](H2O) (OUSe), [C6H6N3][H5O2][(UO2)(2)(SeO4)(3)(H2O)] (BH5USe), [C(6)H6N(3)][H7O3][(UO2)(2)(SO4)(3)(H2O)](H2O) (BH7US), [C6H16N][H5O2][(UO2)(2)(SeO4)(3)(H2O)] (TeH5USe), [C6H18N2][(UO2)(2)(SO4)(3)(H2O)] (TmUS), [H5O2](2)[(UO2)(2)(SeO4)(3)(H2O)](H2O) (H5USe-1), [H5O2](2)[(UO2)(2)(SeO4)(3)(H2O)(2)](H2O)(9) (H5USe-2), and [C4H14N2][(UO2)(2) (SeO4)(3)(H2O)] (H2O) (DmUSe) have been prepared by isothermal evaporation of aqueous solutions containing extra sulfuric or selenic acid. Their crystal structures can be considered as organo-inorganic hybrids constructed of alternating [(UO2)(2)(TO4)(3)(H2O)(n)](2-) slabs (T=Se6+, S6+, n=1, 2) and layers containing templating organic moieties and/or hydronium ions and water molecules. The organic and inorganic parts of the structures are linked by multiple hydrogen bonds. Besides structure description, we offer topological analysis of the inorganic fragments with UO2:TO4 ratio of 23 as modular units resulting from self-assembly of fundamental chains formed by [(UO2)(2)(TO4)(2)] tetramers and TO4 tetrahedra.