La2Ni3C24H30(NO4)6 crystallizes in the trigonal P-3 space group. La(1) is bonded in a 9-coordinate geometry to three equivalent O(1), three equivalent O(3), and three equivalent O(4) atoms. All La(1)-O(1) bond lengths are 2.43 Å. All La(1)-O(3) bond lengths are 2.53 Å. All La(1)-O(4) bond lengths are 2.89 Å. Ni(1) is bonded in an octahedral geometry to two equivalent N(1), two equivalent O(2), and two equivalent O(3) atoms. Both Ni(1)-N(1) bond lengths are 2.00 Å. Both Ni(1)-O(2) bond lengths are 1.94 Å. Both Ni(1)-O(3) bond lengths are 2.32 Å. There are four inequivalent C sites. In the first C site, C(1) is bonded in a distorted bent 120 degrees geometry to one O(1) and one O(2) atom. The C(1)-O(1) bond length is 1.26 Å. The C(1)-O(2) bond length is 1.28 Å. In the second C site, C(2) is bonded in a distorted trigonal non-coplanar geometry to one N(1), one H(1), and one H(2) atom. The C(2)-N(1) bond length is 1.48 Å. The C(2)-H(1) bond length is 1.10 Å. The C(2)-H(2) bond length is 1.10 Å. In the third C site, C(3) is bonded in a distorted trigonal non-coplanar geometry to one N(1), one H(4), and one H(5) atom. The C(3)-N(1) bond length is 1.47 Å. The C(3)-H(4) bond length is 1.10 Å. The C(3)-H(5) bond length is 1.10 Å. In the fourth C site, C(4) is bonded in a distorted bent 120 degrees geometry to one O(3) and one O(4) atom. The C(4)-O(3) bond length is 1.28 Å. The C(4)-O(4) bond length is 1.26 Å. N(1) is bonded to one Ni(1), one C(2), one C(3), and one H(3) atom to form distorted corner-sharing NNiHC2 tetrahedra. The N(1)-H(3) bond length is 1.04 Å. There are five inequivalent H sites. In the first H site, H(1) is bonded in a single-bond geometry to one C(2) atom. In the second H site, H(2) is bonded in a single-bond geometry to one C(2) atom. In the third H site, H(3) is bonded in a single-bond geometry to one N(1) atom. In the fourth H site, H(4) is bonded in a single-bond geometry to one C(3) atom. In the fifth H site, H(5) is bonded in a single-bond geometry to one C(3) atom. There are four inequivalent O sites. In the first O site, O(1) is bonded in a bent 150 degrees geometry to one La(1) and one C(1) atom. In the second O site, O(2) is bonded in a bent 120 degrees geometry to one Ni(1) and one C(1) atom. In the third O site, O(3) is bonded in a distorted single-bond geometry to one La(1), one Ni(1), and one C(4) atom. In the fourth O site, O(4) is bonded in a single-bond geometry to one La(1) and one C(4) atom. Linkers: 6 [O]C(=O)CNCC([O])=O. Metal clusters: 2 [La] ,3 [Ni]. The MOF has largest included sphere 7.25 A, density 1.79 g/cm3, surface area 3073.23 m2/g, accessible volume 0.23 cm3/g