A new compound, Tl₂[(UO₂)₂(MoO ₄)₃], was prepared by a solid-phase reaction. The compound crystallizes in a rhombic system, space group Pna2₁, a = 20.1296(9), b = 8.2811(4), c = 9.7045(4) Å, V = 1617.69(13) ų, Z = 4. The crystal structrue was solved by the direct method and refined to R ₁ = 0. 04 for 4884 unique reflections. The structural motif is a framework consisting of UO₇ pentagonal bipyramids and MoO₄ tetrahedra. The Tl coordination polyhedra are irregular, with seven and eight vertices. Large channels of the size 6 x 10.8 Å, occupied by Tl ⁺ cations, are arranged parallel to the [001] direction. The compound is isostructural to the previously described α-Cs₂(UO ₂)₂(MoO₄)₃ and Rb ₂(UO₂)₂ (MoO₄)₃.