NdCH3SO7 crystallizes in the tetragonal P4_3 space group. Nd(1) is bonded in a 9-coordinate geometry to one O(2), one O(3), one O(4), one O(5), one O(7), two equivalent O(1), and two equivalent O(6) atoms. The Nd(1)-O(2) bond length is 2.44 Å. The Nd(1)-O(3) bond length is 2.36 Å. The Nd(1)-O(4) bond length is 2.52 Å. The Nd(1)-O(5) bond length is 2.49 Å. The Nd(1)-O(7) bond length is 2.46 Å. There is one shorter (2.56 Å) and one longer (2.67 Å) Nd(1)-O(1) bond length. There is one shorter (2.56 Å) and one longer (2.76 Å) Nd(1)-O(6) bond length. C(1) is bonded in a trigonal planar geometry to one H(1), one O(1), and one O(6) atom. The C(1)-H(1) bond length is 1.10 Å. The C(1)-O(1) bond length is 1.28 Å. The C(1)-O(6) bond length is 1.27 Å. There are three inequivalent H sites. In the first H site, H(1) is bonded in a single-bond geometry to one C(1) atom. In the second H site, H(2) is bonded in a distorted single-bond geometry to one O(5) and one O(7) atom. The H(2)-O(5) bond length is 1.69 Å. The H(2)-O(7) bond length is 0.99 Å. In the third H site, H(3) is bonded in a single-bond geometry to one O(7) atom. The H(3)-O(7) bond length is 0.98 Å. S(1) is bonded in a tetrahedral geometry to one O(2), one O(3), one O(4), and one O(5) atom. The S(1)-O(2) bond length is 1.48 Å. The S(1)-O(3) bond length is 1.47 Å. The S(1)-O(4) bond length is 1.48 Å. The S(1)-O(5) bond length is 1.50 Å. There are seven inequivalent O sites. In the first O site, O(3) is bonded in a distorted bent 150 degrees geometry to one Nd(1) and one S(1) atom. In the second O site, O(4) is bonded in a distorted single-bond geometry to one Nd(1) and one S(1) atom. In the third O site, O(5) is bonded in a distorted trigonal planar geometry to one Nd(1), one H(2), and one S(1) atom. In the fourth O site, O(6) is bonded in a distorted single-bond geometry to two equivalent Nd(1) and one C(1) atom. In the fifth O site, O(7) is bonded in a water-like geometry to one Nd(1), one H(2), and one H(3) atom. In the sixth O site, O(1) is bonded in a distorted single-bond geometry to two equivalent Nd(1) and one C(1) atom. In the seventh O site, O(2) is bonded in a distorted bent 150 degrees geometry to one Nd(1) and one S(1) atom. Linkers: 4 [O]C=O ,4 [O]S([O])(=O)=O. Metal clusters: 4 [Nd]. The MOF has largest included sphere 1.40 A, density 3.58 g/cm3, surface area 1529.39 m2/g, accessible volume 0.03 cm3/g