The new uranyl phosphate [(UO2)(3)(PO4)O(OH)(H2O)(2)] (H2O) (1) with an unprecedented framework structure has been synthesized at 150 and 185 degreesC. The structure (tetragonal, P4(2)/mbc, a = 14.015(1) Angstrom, c = 13.083(2) Angstrom, V = 2575.6(4) Angstrom(3), Z = 8) contains uranyl phosphate chains composed of uranyl pentagonal and hexagonal bipyramids and phosphate tetrahedra linked by sharing of polyhedral edges. The uranyl phosphate chains are aligned both along [100] and [010] and are linked into a novel framework structure involving channels along [001]. Topologically identical chains occur linked into sheets in more than a dozen uranyl phosphate minerals, but these chains have never been observed in opposing orientations and linked into a framework as in 1.