Three new uranyl chromate-dichromates, [dabcoH ₂][(UO ₂)(CrO ₄)(Cr ₂O ₇)](H ₂O) ₂ (1), [dmedaH ₂][(UO ₂)(CrO ₄)(Cr ₂O ₇)](H ₂O) (2), and [pyH] ₄[(UO ₂)(CrO ₄) ₂(Cr ₂O ₇)] (3) were prepared by evaporation of aqueous solutions under ambient conditions. Compound 1 is triclinic, P1¯, a = 7.2533(15), b = 10.328(2), c = 12.399(2) Å, α = 89.292(4), β = 88.124(4), γ = 78.753(4)°, V = 910.5(3) Å ³, R ₁ = 0.024; 2is monoclinic, P2 ₁/с, a = 7.315(4), b = 14.684(8), c = 15.812(9) Å, β = 99.696(12)°, V = 1674.2(15) Å ³, R ₁ = 0.034; 3 is orthorhombic, Pnma, a = 16.396(4), b = 21.129(6), c = 7.119(2) Å, V = 2466.1(12) Å ³, R ₁ = 0.045. In the crystal structures of 1 and 2, the UO ₇ bipyramids and CrO ₄ tetrahedra share vertices to form 1∞[(UO ₂)(CrO ₄)] chains; the dichromate groups Cr ₂O ₇decorate them with formation of 1∞[(UO ₂)(CrO ₄)(Cr ₂O ₇)] ²⁻chains. In 3,polymerization of 1∞[(UO ₂)(CrO ₄)(Cr ₂O ₇)] ²⁻chains produced 2∞[(UO ₂)(CrO ₄) ₂(Cr ₂O ₇)] ⁴⁻layers. The protonated organic molecules are located in the interlayer and connect to the inorganic backbones via a system of hydrogen bonds. We discuss the structural peculiarities of uranyl chromate-dichromate complexes and the effects of template nature on their geometrical features.