UP2H2(CO)6 crystallizes in the tetragonal P4_2/nmc space group. U(1) is bonded in a 4-coordinate geometry to two equivalent O(1) and two equivalent O(2) atoms. Both U(1)-O(1) bond lengths are 2.30 Å. Both U(1)-O(2) bond lengths are 2.34 Å. There are three inequivalent C sites. In the first C site, C(1) is bonded in a trigonal planar geometry to one C(2), one C(3), and one P(1) atom. The C(1)-C(2) bond length is 1.39 Å. The C(1)-C(3) bond length is 1.35 Å. The C(1)-P(1) bond length is 1.80 Å. In the second C site, C(2) is bonded in a bent 120 degrees geometry to one C(1) and one C(3) atom. The C(2)-C(3) bond length is 1.39 Å. In the third C site, C(3) is bonded in a distorted single-bond geometry to one C(1), one C(2), and one H(1) atom. The C(3)-H(1) bond length is 0.95 Å. P(1) is bonded in a tetrahedral geometry to one C(1), one O(1), one O(2), and one O(3) atom. The P(1)-O(1) bond length is 1.50 Å. The P(1)-O(2) bond length is 1.49 Å. The P(1)-O(3) bond length is 1.56 Å. H(1) is bonded in a single-bond geometry to one C(3) atom. There are three inequivalent O sites. In the first O site, O(2) is bonded in a distorted single-bond geometry to one U(1) and one P(1) atom. In the second O site, O(3) is bonded in a single-bond geometry to one P(1) atom. In the third O site, O(1) is bonded in a distorted bent 150 degrees geometry to one U(1) and one P(1) atom. Linkers: 8 [O]P([O])(=O)c1[c]cc(P([O])([O])=O)[c]c1. Metal clusters: 8 [U]. The MOF has largest included sphere 9.06 A, density 1.93 g/cm3, surface area 2480.39 m2/g, accessible volume 0.28 cm3/g