The crystals of four amine-templated uranyl oxoselenates(VI), [C ₃H₁₂N₂][(UO₂)(SeO₄) ₂(H₂O)₂](H₂O) (1), [C ₅H₁₆N₂]₂[(UO₂)-(SeO ₄)₂(H₂O)](NO₃)₂ (2), [C₄H₁₂N][(UO₂)(SeO₄)(NO ₃)] (3), and [C₄H₁₄N₂][(UO ₂)(SeO₄)₂(H₂O)] (4) were prepared by evaporation from aqueous solution of uranyl nitrate, selenic acid and the respective amine. The crystal structures of all four compounds have been solved by direct methods from X-ray diffraction data. The structure of 1 (triclinic, P1, a = 7.5611(16), b = 7.7650(17), c = 12.925(3) Å, α = 94.605(18), β = 94.405(17), γ = 96.470(17)°, V = 748.8(3) ų, R₁ = 0.029 for 2769 unique observed reflections) is based upon 0D-units of the composition [(UO₂) ₂(SeO₄)₄(H₂O)₄] ^4-. These discrete units are composed from two pentagonal [UO ₇]^8- bipyramids linked via [SeO₄]^2- tetrahedra and are unknown in structural chemistry of uranium so far. The structure of 2 (monoclinic, C2/c, a = 28.916(5), b = 8.0836(10), c = 11.9856(16) Å, β = 110.909(11)°, V = 2617.1(6) ų, R ₁ = 0.035 for 2578 unique observed reflections) contains [(UO ₂)(SeO₄)₂(H₂O)]^2- chains of corner-sharing pentagonal [UO₇]^8- bipyramids and [SeO₄]^2- tetrahedra. The chains run parallel to the c axis and are arranged into layers parallel to (100). In the structure of 3 (monoclinic, C2/m, a = 21.244(5), b = 7.1092(11), c = 8.6581(18) Å, β = 97.693(17)°, V = 1295.8(4) ų, R₁ = 0.027 for 1386 unique observed reflections), pentagonal [UO₇]^8- bipyramids share corners with three [SeO₄]^2- tetrahedra each and an edge with a [NO₃]^- anion to form [(UO ₂)(SeO₄)(NO₃)]^- chains parallel to the b axis. In the structure of 4 (triclinic, P1, a = 6.853(2), b = 10.537(3), c = 10.574(3) Å, α = 99.62(3), β = 94.45(3), γ = 100.52(3)°, V = 735.6(4) ų, R₁ = 0.045 for 2713 unique observed reflections), one symmetrically independent pentagonal [UO ₇]^8- bipyramid shares corners with four [SeO ₄]^2- tetrahedra to form the [(UO₂)(SeO ₄)₂(H₂O)]^2- chains parallel to the a axis. A comparison to related uranyl compounds is given.