MoNiC20H16(NO)4 crystallizes in the tetragonal P4_12_12 space group. Mo(1) is bonded to one O(1), one O(2), one O(3), and one O(4) atom to form MoO4 tetrahedra that share corners with two equivalent Ni(1)N4O2 octahedra. The corner-sharing octahedral tilt angles range from 25-31°. The Mo(1)-O(1) bond length is 1.76 Å. The Mo(1)-O(2) bond length is 1.80 Å. The Mo(1)-O(3) bond length is 1.76 Å. The Mo(1)-O(4) bond length is 1.80 Å. Ni(1) is bonded to one N(1), one N(2), one N(3), one N(4), one O(2), and one O(4) atom to form NiN4O2 octahedra that share corners with two equivalent Mo(1)O4 tetrahedra. The Ni(1)-N(1) bond length is 2.07 Å. The Ni(1)-N(2) bond length is 2.07 Å. The Ni(1)-N(3) bond length is 2.13 Å. The Ni(1)-N(4) bond length is 2.14 Å. The Ni(1)-O(2) bond length is 2.01 Å. The Ni(1)-O(4) bond length is 2.01 Å. There are twenty inequivalent C sites. In the first C site, C(15) is bonded in a distorted bent 120 degrees geometry to one N(2) and one H(12) atom. The C(15)-N(2) bond length is 1.34 Å. The C(15)-H(12) bond length is 1.09 Å. In the second C site, C(16) is bonded in a distorted bent 120 degrees geometry to one C(17), one N(4), and one H(13) atom. The C(16)-C(17) bond length is 1.39 Å. The C(16)-N(4) bond length is 1.35 Å. The C(16)-H(13) 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 H(1) atom. The C(1)-C(2) bond length is 1.39 Å. The C(1)-N(1) bond length is 1.35 Å. The C(1)-H(1) bond length is 1.09 Å. In the fourth C site, C(17) is bonded in a distorted trigonal planar geometry to one C(16), one C(18), and one H(14) atom. The C(17)-C(18) bond length is 1.39 Å. The C(17)-H(14) bond length is 1.09 Å. In the fifth C site, C(2) is bonded in a distorted trigonal planar geometry to one C(1), one C(3), and one H(2) atom. The C(2)-C(3) bond length is 1.41 Å. The C(2)-H(2) bond length is 1.09 Å. In the sixth C site, C(18) is bonded in a distorted trigonal planar geometry to one C(17), one C(19), and one H(15) atom. The C(18)-C(19) bond length is 1.41 Å. The C(18)-H(15) bond length is 1.09 Å. In the seventh C site, C(3) is bonded in a trigonal planar geometry to one C(19), one C(2), and one C(4) atom. The C(3)-C(19) bond length is 1.48 Å. The C(3)-C(4) bond length is 1.40 Å. In the eighth C site, C(19) is bonded in a trigonal planar geometry to one C(18), one C(20), and one C(3) atom. The C(19)-C(20) bond length is 1.40 Å. In the ninth C site, C(4) is bonded in a distorted single-bond geometry to one C(3) and one H(3) atom. The C(4)-H(3) bond length is 1.09 Å. In the tenth C site, C(20) is bonded in a distorted bent 120 degrees geometry to one C(19), one N(4), and one H(16) atom. The C(20)-N(4) bond length is 1.34 Å. The C(20)-H(16) bond length is 1.09 Å. In the eleventh C site, C(5) is bonded in a distorted bent 120 degrees geometry to one N(1) and one H(4) atom. The C(5)-N(1) bond length is 1.34 Å. The C(5)-H(4) bond length is 1.09 Å. In the twelfth C site, C(6) is bonded in a distorted trigonal planar geometry to one C(7), one N(3), and one H(5) atom. The C(6)-C(7) bond length is 1.39 Å. The C(6)-N(3) bond length is 1.35 Å. The C(6)-H(5) bond length is 1.09 Å. In the thirteenth C site, C(7) is bonded in a distorted trigonal planar geometry to one C(6), one C(8), and one H(6) atom. The C(7)-C(8) bond length is 1.39 Å. The C(7)-H(6) bond length is 1.09 Å. In the fourteenth C site, C(8) is bonded in a distorted trigonal planar geometry to one C(7), one C(9), and one H(7) atom. The C(8)-C(9) bond length is 1.41 Å. The C(8)-H(7) bond length is 1.09 Å. In the fifteenth C site, C(9) is bonded in a trigonal planar geometry to one C(10), one C(13), and one C(8) atom. The C(9)-C(10) bond length is 1.41 Å. The C(9)-C(13) bond length is 1.48 Å. In the sixteenth C site, C(10) is bonded in a distorted bent 120 degrees geometry to one C(9), one N(3), and one H(8) atom. The C(10)-N(3) bond length is 1.34 Å. The C(10)-H(8) bond length is 1.09 Å. In the seventeenth C site, C(11) is bonded in a distorted bent 120 degrees geometry to one C(12), one N(2), and one H(9) atom. The C(11)-C(12) bond length is 1.39 Å. The C(11)-N(2) bond length is 1.35 Å. The C(11)-H(9) bond length is 1.09 Å. In the eighteenth C site, C(14) is bonded in a distorted single-bond geometry to one C(13) and one H(11) atom. The C(14)-C(13) bond length is 1.41 Å. The C(14)-H(11) bond length is 1.09 Å. In the nineteenth C site, C(12) is bonded in a distorted trigonal planar geometry to one C(11), one C(13), and one H(10) atom. The C(12)-C(13) bond length is 1.40 Å. The C(12)-H(10) bond length is 1.09 Å. In the twentieth C site, C(13) is bonded in a trigonal planar geometry to one C(12), one C(14), and one C(9) atom. There are four inequivalent N sites. In the first N site, N(1) is bonded in a trigonal planar geometry to one Ni(1), one C(1), and one C(5) atom. In the second N site, N(2) is bonded in a trigonal planar geometry to one Ni(1), one C(11), and one C(15) atom. In the third N site, N(3) is bonded in a trigonal planar geometry to one Ni(1), one C(10), and one C(6) atom. In the fourth N site, N(4) is bonded in a trigonal planar geometry to one Ni(1), one C(16), and one C(20) atom. There are sixteen inequivalent H sites. In the first H site, H(15) is bonded in a single-bond geometry to one C(18) atom. In the second H site, H(16) is bonded in a single-bond geometry to one C(20) atom. In the third H site, H(1) is bonded in a single-bond geometry to one C(1) atom. In the fourth H site, H(2) is bonded in a single-bond geometry to one C(2) atom. In the fifth H site, H(3) is bonded in a single-bond geometry to one C(4) atom. In the sixth H site, H(4) is bonded in a single-bond geometry to one C(5) atom. In the seventh H site, H(5) is bonded in a single-bond geometry to one C(6) atom. In the eighth H site, H(6) is bonded in a single-bond geometry to one C(7) atom. In the ninth H site, H(7) is bonded in a single-bond geometry to one C(8) atom. In the tenth H site, H(8) is bonded in a single-bond geometry to one C(10) atom. In the eleventh H site, H(9) is bonded in a single-bond geometry to one C(11) atom. In the twelfth H site, H(10) is bonded in a single-bond geometry to one C(12) atom. In the thirteenth H site, H(11) is bonded in a single-bond geometry to one C(14) atom. In the fourteenth H site, H(12) is bonded in a single-bond geometry to one C(15) atom. In the fifteenth H site, H(13) is bonded in a single-bond geometry to one C(16) atom. In the sixteenth H site, H(14) is bonded in a single-bond geometry to one C(17) atom. There are four inequivalent O sites. In the first O site, O(1) is bonded in a single-bond geometry to one Mo(1) atom. In the second O site, O(2) is bonded in a bent 150 degrees geometry to one Mo(1) and one Ni(1) atom. In the third O site, O(3) is bonded in a single-bond geometry to one Mo(1) atom. In the fourth O site, O(4) is bonded in a bent 150 degrees geometry to one Mo(1) and one Ni(1) atom. Linkers: 16 c1cncc(-c2ccncc2)c1. Metal clusters: 8 [Ni] ,8 [Mo]. The MOF has largest included sphere 4.71 A, density 1.39 g/cm3, surface area 3761.52 m2/g, accessible volume 0.26 cm3/g