Gd9C72H37(N6O19)2 crystallizes in the trigonal R-3c space group. There are two inequivalent Gd sites. In the first Gd site, Gd(1) is bonded in a 8-coordinate geometry to one O(2), one O(3), one O(6), one O(7), two equivalent O(1), and two equivalent O(4) atoms. The Gd(1)-O(2) bond length is 2.46 Å. The Gd(1)-O(3) bond length is 2.31 Å. The Gd(1)-O(6) bond length is 2.31 Å. The Gd(1)-O(7) bond length is 2.31 Å. There is one shorter (2.39 Å) and one longer (2.51 Å) Gd(1)-O(1) bond length. There is one shorter (2.41 Å) and one longer (2.47 Å) Gd(1)-O(4) bond length. In the second Gd site, Gd(2) is bonded in a 10-coordinate geometry to two equivalent N(1), two equivalent N(2), two equivalent O(3), two equivalent O(5), and two equivalent O(6) atoms. Both Gd(2)-N(1) bond lengths are 2.65 Å. Both Gd(2)-N(2) bond lengths are 2.56 Å. Both Gd(2)-O(3) bond lengths are 2.51 Å. Both Gd(2)-O(5) bond lengths are 2.35 Å. Both Gd(2)-O(6) bond lengths are 2.50 Å. There are twelve inequivalent C sites. In the first C site, C(10) is bonded in a distorted trigonal planar geometry to one C(11), one C(9), and one H(5) atom. The C(10)-C(11) bond length is 1.40 Å. The C(10)-C(9) bond length is 1.39 Å. The C(10)-H(5) bond length is 1.09 Å. In the second C site, C(11) is bonded in a distorted bent 120 degrees geometry to one C(10), one N(2), and one H(6) atom. The C(11)-N(2) bond length is 1.34 Å. The C(11)-H(6) bond length is 1.09 Å. In the third C site, C(1) is bonded in a distorted bent 120 degrees geometry to one C(2), one N(1), and one O(3) atom. The C(1)-C(2) bond length is 1.42 Å. The C(1)-N(1) bond length is 1.36 Å. The C(1)-O(3) bond length is 1.29 Å. In the fourth C site, C(12) is bonded in a distorted bent 120 degrees geometry to one C(8), one O(4), and one O(5) atom. The C(12)-C(8) bond length is 1.48 Å. The C(12)-O(4) bond length is 1.30 Å. The C(12)-O(5) bond length is 1.26 Å. In the fifth C site, C(2) is bonded in a trigonal planar geometry to one C(1), one C(3), and one C(6) atom. The C(2)-C(3) bond length is 1.40 Å. The C(2)-C(6) bond length is 1.48 Å. In the sixth C site, C(3) is bonded in a distorted trigonal planar geometry to one C(2), one C(4), and one H(1) atom. The C(3)-C(4) bond length is 1.39 Å. The C(3)-H(1) bond length is 1.09 Å. In the seventh C site, C(4) is bonded in a distorted single-bond geometry to one C(3), one C(5), and one H(2) atom. The C(4)-C(5) bond length is 1.40 Å. The C(4)-H(2) bond length is 1.09 Å. In the eighth C site, C(5) is bonded in a distorted trigonal planar geometry to one C(4), one N(1), and one H(3) atom. The C(5)-N(1) bond length is 1.33 Å. The C(5)-H(3) bond length is 1.09 Å. In the ninth C site, C(6) is bonded in a bent 120 degrees geometry to one C(2), one O(1), and one O(2) atom. The C(6)-O(1) bond length is 1.31 Å. The C(6)-O(2) bond length is 1.27 Å. In the tenth C site, C(7) is bonded in a distorted trigonal planar geometry to one C(8), one N(2), and one O(6) atom. The C(7)-C(8) bond length is 1.42 Å. The C(7)-N(2) bond length is 1.36 Å. The C(7)-O(6) bond length is 1.31 Å. In the eleventh C site, C(8) is bonded in a trigonal planar geometry to one C(12), one C(7), and one C(9) atom. The C(8)-C(9) bond length is 1.40 Å. In the twelfth C site, C(9) is bonded in a distorted single-bond geometry to one C(10), one C(8), and one H(4) atom. The C(9)-H(4) bond length is 1.09 Å. There are two inequivalent N sites. In the first N site, N(1) is bonded in a distorted bent 120 degrees geometry to one Gd(2), one C(1), and one C(5) atom. In the second N site, N(2) is bonded in a distorted bent 120 degrees geometry to one Gd(2), one C(11), and one C(7) atom. There are seven inequivalent H sites. In the first H site, H(1) is bonded in a single-bond geometry to one C(3) atom. In the second H site, H(2) is bonded in a single-bond geometry to one C(4) atom. In the third H site, H(3) is bonded in a single-bond geometry to one C(5) atom. In the fourth H site, H(4) is bonded in a single-bond geometry to one C(9) atom. In the fifth H site, H(5) is bonded in a single-bond geometry to one C(10) atom. In the sixth H site, H(6) is bonded in a single-bond geometry to one C(11) atom. In the seventh H site, H(7) is bonded in a linear geometry to two equivalent O(7) atoms. Both H(7)-O(7) bond lengths are 1.22 Å. There are seven inequivalent O sites. In the first O site, O(1) is bonded in a 3-coordinate geometry to two equivalent Gd(1) and one C(6) atom. In the second O site, O(2) is bonded in a distorted L-shaped geometry to one Gd(1) and one C(6) atom. In the third O site, O(3) is bonded in a 3-coordinate geometry to one Gd(1), one Gd(2), and one C(1) atom. In the fourth O site, O(4) is bonded in a distorted trigonal planar geometry to two equivalent Gd(1) and one C(12) atom. In the fifth O site, O(5) is bonded in a distorted bent 150 degrees geometry to one Gd(2) and one C(12) atom. In the sixth O site, O(6) is bonded in a 3-coordinate geometry to one Gd(1), one Gd(2), and one C(7) atom. In the seventh O site, O(7) is bonded to three equivalent Gd(1) and one H(7) atom to form distorted corner-sharing OGd3H tetrahedra. Linkers: 19 [O]C(=O)[C]1C=CC=NC1=O ,5 [O]C(=O)C1=C[CH]C=NC1=O. Metal clusters: 18 [Gd]. The MOF has largest included sphere 6.04 A, density 2.19 g/cm3, surface area 2268.82 m2/g, accessible volume 0.16 cm3/g