V2NiC4H8(N4O3)2 crystallizes in the trigonal R3 space group. V(1,2) is bonded to one O(1), one O(3), one O(4), and one O(5) atom to form VO4 tetrahedra that share  a cornercorner with one Ni(1)N3O3 octahedra and corners with two equivalent V(1,2)O4 tetrahedra. The corner-sharing octahedral tilt angles are 19°. The V(1,2)-O(1) bond length is 1.67 Å. The V(1,2)-O(3) bond length is 1.81 Å. The V(1,2)-O(4) bond length is 1.79 Å. The V(1,2)-O(5) bond length is 1.66 Å. There are three inequivalent Ni sites. In the first Ni site, Ni(1) is bonded to three equivalent N(1) and three equivalent O(1) atoms to form NiN3O3 octahedra that share corners with three equivalent V(1,2)O4 tetrahedra. All Ni(1)-N(1) bond lengths are 2.03 Å. All Ni(1)-O(1) bond lengths are 2.07 Å. In the second Ni site, Ni(2) is bonded to three equivalent N(2) and three equivalent O(2) atoms to form NiN3O3 octahedra that share corners with three equivalent V(1,2)O4 tetrahedra. All Ni(2)-N(2) bond lengths are 2.03 Å. All Ni(2)-O(2) bond lengths are 2.06 Å. In the third Ni site, Ni(3) is bonded in an octahedral geometry to three equivalent N(3) and three equivalent N(4) atoms. All Ni(3)-N(3) bond lengths are 2.07 Å. All Ni(3)-N(4) bond lengths are 2.07 Å. There are four inequivalent C sites. In the first C site, C(1) is bonded in a trigonal planar geometry to one N(1), one N(5), and one N(7) atom. The C(1)-N(1) bond length is 1.34 Å. The C(1)-N(5) bond length is 1.37 Å. The C(1)-N(7) bond length is 1.34 Å. In the second C site, C(2) is bonded in a trigonal planar geometry to one N(2), one N(6), and one N(8) atom. The C(2)-N(2) bond length is 1.34 Å. The C(2)-N(6) bond length is 1.37 Å. The C(2)-N(8) bond length is 1.34 Å. In the third C site, C(3) is bonded in a trigonal planar geometry to one N(3), one N(5), and one H(1) atom. The C(3)-N(3) bond length is 1.31 Å. The C(3)-N(5) bond length is 1.37 Å. The C(3)-H(1) bond length is 1.08 Å. In the fourth C site, C(4) is bonded in a trigonal planar geometry to one N(4), one N(6), and one H(2) atom. The C(4)-N(4) bond length is 1.31 Å. The C(4)-N(6) bond length is 1.36 Å. The C(4)-H(2) bond length is 1.08 Å. There are eight inequivalent N sites. In the first N site, N(1) is bonded in a distorted trigonal planar geometry to one Ni(1), one C(1), and one N(3) atom. The N(1)-N(3) bond length is 1.38 Å. In the second N site, N(2) is bonded in a distorted trigonal planar geometry to one Ni(2), one C(2), and one N(4) atom. The N(2)-N(4) bond length is 1.38 Å. In the third N site, N(3) is bonded in a distorted trigonal planar geometry to one Ni(3), one C(3), and one N(1) atom. In the fourth N site, N(4) is bonded in a distorted trigonal planar geometry to one Ni(3), one C(4), and one N(2) atom. In the fifth N site, N(5) is bonded in a trigonal planar geometry to one C(1), one C(3), and one H(3) atom. The N(5)-H(3) bond length is 1.02 Å. In the sixth N site, N(6) is bonded in a trigonal planar geometry to one C(2), one C(4), and one H(4) atom. The N(6)-H(4) bond length is 1.02 Å. In the seventh N site, N(7) is bonded in a distorted trigonal planar geometry to one C(1); one H(5); and one H(7,8) atom. The N(7)-H(5) bond length is 1.02 Å. The N(7)-H(7,8) bond length is 1.04 Å. In the eighth N site, N(8) is bonded in a distorted trigonal planar geometry to one C(2); one H(6); and one H(7,8) atom. The N(8)-H(6) bond length is 1.02 Å. The N(8)-H(7,8) bond length is 1.04 Å. 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 N(5) atom. In the fourth H site, H(4) is bonded in a single-bond geometry to one N(6) atom. In the fifth H site, H(5) is bonded in a single-bond geometry to one N(7) atom. In the sixth H site, H(6) is bonded in a single-bond geometry to one N(8) atom. In the seventh H site, H(7,8) is bonded in a distorted single-bond geometry to one N(7) and one O(6) atom. The H(7,8)-O(6) bond length is 1.71 Å. There are six inequivalent O sites. In the first O site, O(1) is bonded in a distorted bent 150 degrees geometry to one V(1,2) and one Ni(1) atom. In the second O site, O(2) is bonded in a distorted bent 150 degrees geometry to one V(1,2) and one Ni(2) atom. The O(2)-V(1,2) bond length is 1.67 Å. In the third O site, O(3) is bonded in a bent 150 degrees geometry to two equivalent V(1,2) atoms. In the fourth O site, O(4) is bonded in a bent 150 degrees geometry to two equivalent V(1,2) atoms. In the fifth O site, O(5) is bonded in a distorted single-bond geometry to one V(1,2) and one H(7,8) atom. The O(5)-H(7,8) bond length is 1.71 Å. In the sixth O site, O(6) is bonded in a distorted single-bond geometry to one V(1,2) and one H(7,8) atom. The O(6)-V(1,2) bond length is 1.66 Å. Linkers: 6 Nc1nnc[nH]1. Metal clusters: 6 [V] ,3 [Ni]. The MOF has largest included sphere 2.46 A, density 2.09 g/cm3, surface area 2984.85 m2/g, accessible volume 0.11 cm3/g