Four novel uranyl silicates and germanates with framework structures, K4Na2(UO2)(3)(Si2O7)(2)-3H(2)O, K4Na2(UO2)(3)(Ge2O7)(2)center dot 3H(2)O, H3O(UO2)(2)(HGe2O7)center dot 2H(2)O, and Na-2(UO2)GeO4, have been synthesized by means of the hydrothermal method. The structures of the title compounds were refined by single-crystal X-ray diffraction and characterized by Raman spectroscopy. We used the method of secondary building units (SBUs) for a crystal chemical analysis of the 3D framework and their topologies. The framework of the K4Na2(UO2)(3)(T2O7)(2)center dot 3H(2)O (T = Si, Ge) series exhibits large 14-membered rings and smaller 8- membered rings which are built upon [UT4] pentamers. The internal size of the largest pores is approximately 12.39 x 3.33 <(A) over circle>(2). H3O- (UO2)(2)(HGe2O7)-2H(2)O is based on 10-membered rings with intermediate sized pores. They are built upon [U2Ge2] tetramers with 7-fold-coordinated U. The internal dimension of the pores in H3O(UO2)(2)(HGe2O7)center dot 2H(2)O is smaller compared to the K4Na2(UO2)(3)(T2O7)(2)center dot 3H(2)O (T = Si, Ge) series with similar to 5.91 X 5.33 <(A) over circle>(2). Its topology is similar to several uranium germanate synthetic phases and silicate minerals, especially alpha- and beta-uranophane which are constructed from similar building units. A novel 3D framework type of Na-2(UO2)GeO4 with 8-membered rings demonstrates the smallest free volume in the family of porous uranium germanates. It crystallizes in tetragonal symmetry and is built upon corner sharing of [UGe4] pentamers. The size of the channels is similar to 6.76 x 4.27 <(A) over circle>(2). The vibrational bands in Raman spectra were associated with pyro-(Si2O7)(6-) and -(Ge2O7)(6-) groups, with the Ge-OH bond and with H3O+ cations, confirming the results of the X-ray crystallographic structural characterization. We systemized existing uranyl silicates and germanates based on their building units and chemical composition. We found a simple structural dependence between synthetic conditions and chemical composition.