Ni2C53H68(N3O2)4 crystallizes in the tetragonal P-4b2 space group. Ni(1) is bonded to two equivalent N(1), two equivalent N(3), and two equivalent O(1) atoms to form NiN4O2 octahedra that share corners with two equivalent C(13)H2N2 tetrahedra and corners with two equivalent C(14)H2N2 tetrahedra. Both Ni(1)-N(1) bond lengths are 2.14 Å. Both Ni(1)-N(3) bond lengths are 2.06 Å. Both Ni(1)-O(1) bond lengths are 2.09 Å. There are fourteen inequivalent C sites. In the first C site, C(1) is bonded in a tetrahedral geometry to four equivalent C(2) atoms. All C(1)-C(2) bond lengths are 1.54 Å. In the second C site, C(2) is bonded in a trigonal planar geometry to one C(1), one C(3), and one C(4) atom. The C(2)-C(3) bond length is 1.40 Å. The C(2)-C(4) bond length is 1.41 Å. In the third C site, C(3) is bonded in a distorted single-bond geometry to one C(2), one C(7), and one H(2) atom. The C(3)-C(7) bond length is 1.40 Å. The C(3)-H(2) bond length is 1.09 Å. In the fourth C site, C(4) is bonded in a distorted single-bond geometry to one C(2), one C(5), and one H(3) atom. The C(4)-C(5) bond length is 1.39 Å. The C(4)-H(3) bond length is 1.09 Å. In the fifth C site, C(5) is bonded in a distorted trigonal planar geometry to one C(4), one C(6), and one H(4) atom. The C(5)-C(6) bond length is 1.40 Å. The C(5)-H(4) bond length is 1.09 Å. In the sixth C site, C(6) is bonded in a trigonal planar geometry to one C(5), one C(7), and one C(8) atom. The C(6)-C(7) bond length is 1.40 Å. The C(6)-C(8) bond length is 1.50 Å. In the seventh C site, C(7) is bonded in a distorted trigonal planar geometry to one C(3), one C(6), and one H(5) atom. The C(7)-H(5) bond length is 1.09 Å. In the eighth C site, C(8) is bonded in a distorted bent 120 degrees geometry to one C(6), one O(1), and one O(2) atom. The C(8)-O(1) bond length is 1.29 Å. The C(8)-O(2) bond length is 1.26 Å. In the ninth C site, C(9) is bonded in a distorted trigonal non-coplanar geometry to one N(2), one H(6), and one H(7) atom. The C(9)-N(2) bond length is 1.48 Å. The C(9)-H(6) bond length is 1.10 Å. The C(9)-H(7) bond length is 1.10 Å. In the tenth C site, C(10) is bonded in a distorted trigonal non-coplanar geometry to one N(1), one H(8), and one H(9) atom. The C(10)-N(1) bond length is 1.48 Å. The C(10)-H(8) bond length is 1.09 Å. The C(10)-H(9) bond length is 1.11 Å. In the eleventh C site, C(11) is bonded in a distorted trigonal non-coplanar geometry to one N(1), one H(10), and one H(11) atom. The C(11)-N(1) bond length is 1.47 Å. The C(11)-H(10) bond length is 1.10 Å. The C(11)-H(11) bond length is 1.11 Å. In the twelfth C site, C(12) is bonded in a distorted trigonal non-coplanar geometry to one N(3), one H(12), and one H(13) atom. The C(12)-N(3) bond length is 1.47 Å. The C(12)-H(12) bond length is 1.11 Å. The C(12)-H(13) bond length is 1.10 Å. In the thirteenth C site, C(13) is bonded to one N(2), one N(3), one H(14), and one H(15) atom to form CH2N2 tetrahedra that share  a cornercorner with one Ni(1)N4O2 octahedra and  a cornercorner with one C(14)H2N2 tetrahedra. The corner-sharing octahedral tilt angles are 64°. The C(13)-N(2) bond length is 1.46 Å. The C(13)-N(3) bond length is 1.48 Å. The C(13)-H(14) bond length is 1.11 Å. The C(13)-H(15) bond length is 1.10 Å. In the fourteenth C site, C(14) is bonded to one N(1), one N(2), one H(16), and one H(17) atom to form CH2N2 tetrahedra that share  a cornercorner with one Ni(1)N4O2 octahedra and  a cornercorner with one C(13)H2N2 tetrahedra. The corner-sharing octahedral tilt angles are 72°. The C(14)-N(1) bond length is 1.50 Å. The C(14)-N(2) bond length is 1.45 Å. The C(14)-H(16) bond length is 1.09 Å. The C(14)-H(17) bond length is 1.11 Å. There are three inequivalent N sites. In the first N site, N(3) is bonded in a 4-coordinate geometry to one Ni(1), one C(12), one C(13), and one H(1) atom. The N(3)-H(1) bond length is 1.05 Å. In the second N site, N(1) is bonded to one Ni(1), one C(10), one C(11), and one C(14) atom to form corner-sharing NNiC3 tetrahedra. In the third N site, N(2) is bonded in a trigonal non-coplanar geometry to one C(13), one C(14), and one C(9) atom. There are seventeen inequivalent H sites. In the first H site, H(1) is bonded in a single-bond geometry to one N(3) atom. In the second H site, H(17) is bonded in a single-bond geometry to one C(14) atom. In the third H site, H(2) is bonded in a single-bond geometry to one C(3) atom. In the fourth H site, H(3) is bonded in a single-bond geometry to one C(4) atom. In the fifth H site, H(4) is bonded in a single-bond geometry to one C(5) atom. In the sixth H site, H(5) is bonded in a single-bond geometry to one C(7) atom. In the seventh H site, H(6) is bonded in a single-bond geometry to one C(9) atom. In the eighth H site, H(7) is bonded in a single-bond geometry to one C(9) atom. In the ninth H site, H(8) is bonded in a single-bond geometry to one C(10) atom. In the tenth H site, H(9) is bonded in a single-bond geometry to one C(10) atom. In the eleventh H site, H(10) is bonded in a single-bond geometry to one C(11) atom. In the twelfth H site, H(11) is bonded in a single-bond geometry to one C(11) atom. In the thirteenth H site, H(12) is bonded in a single-bond geometry to one C(12) atom. In the fourteenth H site, H(13) is bonded in a single-bond geometry to one C(12) atom. In the fifteenth H site, H(14) is bonded in a single-bond geometry to one C(13) atom. In the sixteenth H site, H(15) is bonded in a single-bond geometry to one C(13) atom. In the seventeenth H site, H(16) is bonded in a single-bond geometry to one C(14) atom. There are two inequivalent O sites. In the first O site, O(1) is bonded in a distorted bent 120 degrees geometry to one Ni(1) and one C(8) atom. In the second O site, O(2) is bonded in a single-bond geometry to one C(8) atom. Linkers: 4 C1CNC[N@]2CC[N@](CC[N@]3CC[N@](CN1)C3)C2 ,2 [O]C(=O)c1ccc(C(c2ccc(C([O])=O)cc2)(c2ccc(C([O])=O)cc2)c2ccc(C([O])=O)cc2)cc1. Metal clusters: 4 [NH][Ni]([NH])(O[C]=O)O[C]=O. The MOF has largest included sphere 5.77 A, density 1.10 g/cm3, surface area 4818.88 m2/g, accessible volume 0.38 cm3/g