U6(SO4)7 crystallizes in the orthorhombic C222_1 space group. There are three inequivalent U sites. In the first U site, U(1) is bonded in a pentagonal planar geometry to one O(1), one O(2), one O(3), one O(4), and one O(5) atom. The U(1)-O(1) bond length is 2.38 Å. The U(1)-O(2) bond length is 2.33 Å. The U(1)-O(3) bond length is 2.42 Å. The U(1)-O(4) bond length is 2.42 Å. The U(1)-O(5) bond length is 2.38 Å. In the second U site, U(2) is bonded in a 4-coordinate geometry to one O(6), one O(7), one O(8), and one O(9) atom. The U(2)-O(6) bond length is 2.36 Å. The U(2)-O(7) bond length is 2.39 Å. The U(2)-O(8) bond length is 2.38 Å. The U(2)-O(9) bond length is 2.38 Å. In the third U site, U(3) is bonded in a pentagonal planar geometry to one O(10), one O(11), one O(12), one O(13), and one O(14) atom. The U(3)-O(10) bond length is 2.39 Å. The U(3)-O(11) bond length is 2.39 Å. The U(3)-O(12) bond length is 2.39 Å. The U(3)-O(13) bond length is 2.37 Å. The U(3)-O(14) bond length is 2.44 Å. There are four inequivalent S sites. In the first S site, S(1) is bonded in a tetrahedral geometry to one O(1), one O(12), one O(7), and one O(8) atom. The S(1)-O(1) bond length is 1.48 Å. The S(1)-O(12) bond length is 1.48 Å. The S(1)-O(7) bond length is 1.46 Å. The S(1)-O(8) bond length is 1.48 Å. In the second S site, S(2) is bonded in a tetrahedral geometry to one O(10), one O(11), one O(2), and one O(4) atom. The S(2)-O(10) bond length is 1.47 Å. The S(2)-O(11) bond length is 1.47 Å. The S(2)-O(2) bond length is 1.47 Å. The S(2)-O(4) bond length is 1.46 Å. In the third S site, S(3) is bonded in a tetrahedral geometry to one O(14), one O(3), one O(5), and one O(9) atom. The S(3)-O(14) bond length is 1.47 Å. The S(3)-O(3) bond length is 1.46 Å. The S(3)-O(5) bond length is 1.46 Å. The S(3)-O(9) bond length is 1.48 Å. In the fourth S site, S(4) is bonded in a tetrahedral geometry to two equivalent O(13) and two equivalent O(6) atoms. Both S(4)-O(13) bond lengths are 1.47 Å. Both S(4)-O(6) bond lengths are 1.44 Å. There are fourteen inequivalent O sites. In the first O site, O(1) is bonded in a distorted single-bond geometry to one U(1) and one S(1) atom. In the second O site, O(2) is bonded in a distorted linear geometry to one U(1) and one S(2) atom. In the third O site, O(3) is bonded in a distorted single-bond geometry to one U(1) and one S(3) atom. In the fourth O site, O(4) is bonded in a single-bond geometry to one U(1) and one S(2) atom. In the fifth O site, O(5) is bonded in a distorted bent 150 degrees geometry to one U(1) and one S(3) atom. In the sixth O site, O(6) is bonded in a distorted single-bond geometry to one U(2) and one S(4) atom. In the seventh O site, O(7) is bonded in a distorted single-bond geometry to one U(2) and one S(1) atom. In the eighth O site, O(8) is bonded in a distorted single-bond geometry to one U(2) and one S(1) atom. In the ninth O site, O(9) is bonded in a distorted single-bond geometry to one U(2) and one S(3) atom. In the tenth O site, O(10) is bonded in a distorted single-bond geometry to one U(3) and one S(2) atom. In the eleventh O site, O(11) is bonded in a single-bond geometry to one U(3) and one S(2) atom. In the twelfth O site, O(12) is bonded in a distorted single-bond geometry to one U(3) and one S(1) atom. In the thirteenth O site, O(13) is bonded in a distorted single-bond geometry to one U(3) and one S(4) atom. In the fourteenth O site, O(14) is bonded in a distorted single-bond geometry to one U(3) and one S(3) atom. Linkers: 28 [O]S([O])(=O)=O. Metal clusters: 24 [U]. The MOF has largest included sphere 6.44 A, density 3.20 g/cm3, surface area 1346.29 m2/g, accessible volume 0.16 cm3/g