UO2(CsC6NH6O6)2(CH)2 crystallizes in the triclinic P-1 space group. The structure consists of two 02329_fluka molecules and one pitchblend, uranium(iv) oxide, uranium(iv) dioxide, uranium dioxide molecule inside a CsC6NH6O6 framework. In the CsC6NH6O6 framework, Cs(1) is bonded in a 12-coordinate geometry to one H(1), one H(2), one H(3), one H(4), one H(7), one O(1), one O(3), one O(4), one O(6), one O(7), and two equivalent O(2) atoms. The Cs(1)-H(1) bond length is 3.21 Å. The Cs(1)-H(2) bond length is 3.27 Å. The Cs(1)-H(3) bond length is 3.11 Å. The Cs(1)-H(4) bond length is 3.26 Å. The Cs(1)-H(7) bond length is 3.23 Å. The Cs(1)-O(1) bond length is 3.23 Å. The Cs(1)-O(3) bond length is 3.21 Å. The Cs(1)-O(4) bond length is 3.34 Å. The Cs(1)-O(6) bond length is 3.21 Å. The Cs(1)-O(7) bond length is 3.05 Å. There is one shorter (3.09 Å) and one longer (3.45 Å) Cs(1)-O(2) bond length. There are six inequivalent C sites. In the first C site, C(1) is bonded in a distorted trigonal planar geometry to one C(2), one C(6), and one N(1) atom. The C(1)-C(2) bond length is 1.40 Å. The C(1)-C(6) bond length is 1.50 Å. The C(1)-N(1) bond length is 1.35 Å. In the second C site, C(2) is bonded in a distorted single-bond geometry to one C(1) and one H(5) atom. The C(2)-H(5) bond length is 1.09 Å. In the third C site, C(4) is bonded in a distorted single-bond geometry to one C(5) and one H(7) atom. The C(4)-C(5) bond length is 1.40 Å. The C(4)-H(7) bond length is 1.09 Å. In the fourth C site, C(5) is bonded in a distorted trigonal planar geometry to one C(4), one C(7), and one N(1) atom. The C(5)-C(7) bond length is 1.50 Å. The C(5)-N(1) bond length is 1.34 Å. In the fifth C site, C(6) is bonded in a distorted bent 120 degrees geometry to one C(1), one O(1), and one O(2) atom. The C(6)-O(1) bond length is 1.29 Å. The C(6)-O(2) bond length is 1.25 Å. In the sixth C site, C(7) is bonded in a distorted bent 120 degrees geometry to one C(5), one O(3), and one O(4) atom. The C(7)-O(3) bond length is 1.28 Å. The C(7)-O(4) bond length is 1.26 Å. N(1) is bonded in a distorted bent 120 degrees geometry to one C(1) and one C(5) atom. There are six inequivalent H sites. In the first H site, H(1) is bonded in a single-bond geometry to one Cs(1) and one O(6) atom. The H(1)-O(6) bond length is 0.98 Å. In the second H site, H(2) is bonded in a single-bond geometry to one Cs(1) and one O(6) atom. The H(2)-O(6) bond length is 0.98 Å. In the third H site, H(3) is bonded in a single-bond geometry to one Cs(1) and one O(7) atom. The H(3)-O(7) bond length is 0.99 Å. In the fourth H site, H(4) is bonded in a single-bond geometry to one Cs(1) and one O(7) atom. The H(4)-O(7) bond length is 0.98 Å. In the fifth H site, H(5) is bonded in a single-bond geometry to one C(2) atom. In the sixth H site, H(7) is bonded in a single-bond geometry to one Cs(1) and one C(4) atom. There are six inequivalent O sites. In the first O site, O(1) is bonded in a distorted single-bond geometry to one Cs(1) and one C(6) atom. In the second O site, O(2) is bonded in a distorted single-bond geometry to two equivalent Cs(1) and one C(6) atom. In the third O site, O(3) is bonded in a distorted single-bond geometry to one Cs(1) and one C(7) atom. In the fourth O site, O(4) is bonded in a single-bond geometry to one Cs(1) and one C(7) atom. In the fifth O site, O(6) is bonded in a water-like geometry to one Cs(1), one H(1), and one H(2) atom. In the sixth O site, O(7) is bonded in a water-like geometry to one Cs(1), one H(3), and one H(4) atom. Linkers: 2 [O]C(=O)c1cccc(C([O])=O)n1 ,4 O. Metal clusters: 2 [Cs] ,1 [U]. The MOF has largest included sphere 1.74 A, density 2.85 g/cm3, surface area 2620.07 m2/g, accessible volume 0.08 cm3/g