Two new U(VI) compounds templated with organic molecules, [(CH ₆N) ₃(H ₂O)][(CH ₆N) ₂(C ₃H ₁₀N)· (H ₂O)][(UO ₂) ₅(CrO ₄) ₈(H ₂O)] (1) and [(C ₆H ₁₀N ₃O ₃)(H ₅O ₂) ₂(H ₂O)][(H ₅O ₂) ₃(H ₂O)][(UO ₂) ₅(SO ₄) ₈(H ₂O)] (2), were prepared by combination of hydrothermal synthesis and isothermal evaporation methods. Compounds 1 and 2 crystallize in the monoclinic system, space group P2 ₁/n, a = 21.921(5), b = 11.016(2), c = 22.021(5) Å, β = 90.571(5)° for 1 and P ₂/c, a = 18.1693(17), b = 10.0732(10), c = 30.098(3) Å, β = 103.427(2)° for 2. The reflections from the single crystals were collected at 100 K. The structures were solved by the direct methods and refined to R ₁ = 0.053 and 0.070 for 1 and 2, respectively. The crystal structures of 1 and 2 are based on [(UO ₂) ₅(TO ₄) ₈(H ₂O)] ^6– modular layers (T = S ⁶⁺, Cr ⁶⁺) between which protonated organic molecules, water molecules, and hydroxonium ions are located. Specific features of the crystal chemistry of U(VI) compounds with tetrahedral oxoanions with the ratio UO ₂: TO ₄ = 5: 8 (T = S ⁶⁺, Cr ⁶⁺, Se ⁶⁺, Mo ⁶⁺) are considered.