Gd2Ni3H36(C2O3)12 crystallizes in the hexagonal P6/mcc space group. Gd(1) is bonded in a 9-coordinate geometry to three equivalent O(4) and six equivalent O(3) atoms. All Gd(1)-O(4) bond lengths are 2.49 Å. All Gd(1)-O(3) bond lengths are 2.41 Å. Ni(1) is bonded in an octahedral geometry to two equivalent O(1) and four equivalent O(2) atoms. Both Ni(1)-O(1) bond lengths are 2.12 Å. All Ni(1)-O(2) bond lengths are 2.04 Å. There are two inequivalent C sites. In the first C site, C(2) is bonded in a distorted trigonal non-coplanar geometry to one H(2), one H(3), and one O(4) atom. The C(2)-H(2) bond length is 1.11 Å. The C(2)-H(3) bond length is 1.10 Å. The C(2)-O(4) bond length is 1.42 Å. In the second C site, C(1) is bonded in a distorted bent 120 degrees geometry to one O(2) and one O(3) atom. The C(1)-O(2) bond length is 1.25 Å. The C(1)-O(3) bond length is 1.28 Å. There are three inequivalent H sites. In the first H site, H(2) is bonded in a single-bond geometry to one C(2) atom. In the second H site, H(1) is bonded in a single-bond geometry to one O(1) atom. The H(1)-O(1) bond length is 0.99 Å. In the third H site, H(3) is bonded in a single-bond geometry to one C(2) atom. There are four inequivalent O sites. In the first O site, O(1) is bonded in a distorted water-like geometry to one Ni(1) and two equivalent H(1) atoms. In the second O site, O(3) is bonded in a distorted single-bond geometry to one Gd(1) and one C(1) atom. In the third O site, O(2) is bonded in a bent 120 degrees geometry to one Ni(1) and one C(1) atom. In the fourth O site, O(4) is bonded in a distorted bent 120 degrees geometry to one Gd(1) and two equivalent C(2) atoms. Linkers: 12 [O]C(=O)COCC([O])=O. Metal clusters: 4 [Gd] ,6 [Ni]. The MOF has largest included sphere 7.96 A, density 1.62 g/cm3, surface area 3138.83 m2/g, accessible volume 0.28 cm3/g