MoNi2H60(C9N4)4(CH3)4 crystallizes in the monoclinic C2/c space group. The structure consists of sixteen 02329_fluka molecules inside a MoNi2H60(C9N4)4 framework. In the MoNi2H60(C9N4)4 framework, Mo(1) is bonded in a 8-coordinate geometry to two equivalent C(1), two equivalent C(18), two equivalent C(19), and two equivalent C(20) atoms. Both Mo(1)-C(1) bond lengths are 2.14 Å. Both Mo(1)-C(18) bond lengths are 2.13 Å. Both Mo(1)-C(19) bond lengths are 2.17 Å. Both Mo(1)-C(20) bond lengths are 2.17 Å. There are two inequivalent Ni sites. In the first Ni site, Ni(1) is bonded to two equivalent N(1), two equivalent N(2), and two equivalent N(5) atoms to form NiN6 octahedra that share corners with two equivalent C(6)C3N tetrahedra. Both Ni(1)-N(1) bond lengths are 2.10 Å. Both Ni(1)-N(2) bond lengths are 2.05 Å. Both Ni(1)-N(5) bond lengths are 2.06 Å. In the second Ni site, Ni(2) is bonded to two equivalent N(3), two equivalent N(4), and two equivalent N(8) atoms to form NiN6 octahedra that share corners with two equivalent C(14)C3N tetrahedra. Both Ni(2)-N(3) bond lengths are 2.09 Å. Both Ni(2)-N(4) bond lengths are 2.06 Å. Both Ni(2)-N(8) bond lengths are 2.08 Å. There are eighteen inequivalent C sites. In the first C site, C(1) is bonded in a distorted single-bond geometry to one Mo(1) and one N(8) atom. The C(1)-N(8) bond length is 1.15 Å. In the second C site, C(2) is bonded in a 3-coordinate geometry to one N(1) and two equivalent H(5,6) atoms. The C(2)-N(1) bond length is 1.47 Å. Both C(2)-H(5,6) bond lengths are 0.99 Å. In the third C site, C(3) is bonded in a 3-coordinate geometry to one N(2) and two equivalent H(7,8) atoms. The C(3)-N(2) bond length is 1.48 Å. Both C(3)-H(7,8) bond lengths are 0.99 Å. In the fourth C site, C(4) is bonded in a distorted water-like geometry to one N(2) and one H(9) atom. The C(4)-N(2) bond length is 1.33 Å. The C(4)-H(9) bond length is 1.00 Å. In the fifth C site, C(5) is bonded in a water-like geometry to one C(6) and two equivalent H(10,11) atoms. The C(5)-C(6) bond length is 1.53 Å. Both C(5)-H(10,11) bond lengths are 0.99 Å. In the sixth C site, C(6) is bonded to one C(5), one C(8), one C(9), and one N(1) atom to form distorted CC3N tetrahedra that share  a cornercorner with one Ni(1)N6 octahedra. The corner-sharing octahedral tilt angles are 60°. The C(6)-C(8) bond length is 1.53 Å. The C(6)-C(9) bond length is 1.54 Å. The C(6)-N(1) bond length is 1.50 Å. In the seventh C site, C(8) is bonded in a trigonal non-coplanar geometry to one C(6); one H(15,18,19,20); and two equivalent H(16,17) atoms. The C(8)-H(15,18,19,20) bond length is 0.98 Å. Both C(8)-H(16,17) bond lengths are 0.98 Å. In the eighth C site, C(9) is bonded in a trigonal non-coplanar geometry to one C(6) and three equivalent H(15,18,19,20) atoms. All C(9)-H(15,18,19,20) bond lengths are 0.98 Å. In the ninth C site, C(10) is bonded in a 3-coordinate geometry to one N(3) and two equivalent H(21,22) atoms. The C(10)-N(3) bond length is 1.48 Å. Both C(10)-H(21,22) bond lengths are 0.99 Å. In the tenth C site, C(11) is bonded in a 3-coordinate geometry to one N(4) and two equivalent H(23,24) atoms. The C(11)-N(4) bond length is 1.47 Å. Both C(11)-H(23,24) bond lengths are 0.99 Å. In the eleventh C site, C(12) is bonded in a distorted water-like geometry to one N(4) and one H(25) atom. The C(12)-N(4) bond length is 1.32 Å. The C(12)-H(25) bond length is 1.00 Å. In the twelfth C site, C(13) is bonded in a water-like geometry to one C(14) and two equivalent H(26,27) atoms. The C(13)-C(14) bond length is 1.54 Å. Both C(13)-H(26,27) bond lengths are 0.99 Å. In the thirteenth C site, C(14) is bonded to one C(13), one C(16), one C(17), and one N(3) atom to form distorted CC3N tetrahedra that share  a cornercorner with one Ni(2)N6 octahedra. The corner-sharing octahedral tilt angles are 61°. The C(14)-C(16) bond length is 1.54 Å. The C(14)-C(17) bond length is 1.52 Å. The C(14)-N(3) bond length is 1.50 Å. In the fourteenth C site, C(16) is bonded in a trigonal non-coplanar geometry to one C(14); one H(31,34,35,36); and two equivalent H(32,33) atoms. The C(16)-H(31,34,35,36) bond length is 0.98 Å. Both C(16)-H(32,33) bond lengths are 0.98 Å. In the fifteenth C site, C(17) is bonded in a trigonal non-coplanar geometry to one C(14) and three equivalent H(31,34,35,36) atoms. All C(17)-H(31,34,35,36) bond lengths are 0.98 Å. In the sixteenth C site, C(18) is bonded in a distorted single-bond geometry to one Mo(1) and one N(5) atom. The C(18)-N(5) bond length is 1.14 Å. In the seventeenth C site, C(19) is bonded in a distorted linear geometry to one Mo(1) and one N(6) atom. The C(19)-N(6) bond length is 1.16 Å. In the eighteenth C site, C(20) is bonded in a distorted single-bond geometry to one Mo(1) and one N(7) atom. The C(20)-N(7) bond length is 1.16 Å. There are eight inequivalent N sites. In the first N site, N(1) is bonded in a distorted single-bond geometry to one Ni(1), one C(2), one C(6), and one H(1) atom. The N(1)-H(1) bond length is 0.93 Å. In the second N site, N(2) is bonded in a 1-coordinate geometry to one Ni(1), one C(3), one C(4), and one H(2) atom. The N(2)-H(2) bond length is 0.93 Å. In the third N site, N(3) is bonded in a distorted single-bond geometry to one Ni(2), one C(10), one C(14), and one H(3) atom. The N(3)-H(3) bond length is 0.93 Å. In the fourth N site, N(4) is bonded in a 1-coordinate geometry to one Ni(2), one C(11), one C(12), and one H(4) atom. The N(4)-H(4) bond length is 0.93 Å. In the fifth N site, N(5) is bonded in a distorted bent 150 degrees geometry to one Ni(1) and one C(18) atom. In the sixth N site, N(6) is bonded in a single-bond geometry to one C(19) atom. In the seventh N site, N(7) is bonded in a single-bond geometry to one C(20) atom. In the eighth N site, N(8) is bonded in a bent 150 degrees geometry to one Ni(2) and one C(1) atom. There are sixteen inequivalent H sites. In the first H site, H(1) is bonded in a single-bond geometry to one N(1) atom. In the second H site, H(2) is bonded in a single-bond geometry to one N(2) atom. In the third H site, H(3) is bonded in a single-bond geometry to one N(3) atom. In the fourth H site, H(4) is bonded in a single-bond geometry to one N(4) atom. In the fifth H site, H(5,6) is bonded in a single-bond geometry to one C(2) atom. In the sixth H site, H(7,8) is bonded in a single-bond geometry to one C(3) atom. In the seventh H site, H(9) is bonded in a single-bond geometry to one C(4) atom. In the eighth H site, H(10,11) is bonded in a single-bond geometry to one C(5) atom. In the ninth H site, H(15,18,19,20) is bonded in a single-bond geometry to one C(8) atom. In the tenth H site, H(16,17) is bonded in a single-bond geometry to one C(8) atom. In the eleventh H site, H(21,22) is bonded in a single-bond geometry to one C(10) atom. In the twelfth H site, H(23,24) is bonded in a single-bond geometry to one C(11) atom. In the thirteenth H site, H(25) is bonded in a single-bond geometry to one C(12) atom. In the fourteenth H site, H(26,27) is bonded in a single-bond geometry to one C(13) atom. In the fifteenth H site, H(31,34,35,36) is bonded in a single-bond geometry to one C(16) atom. In the sixteenth H site, H(32,33) is bonded in a single-bond geometry to one C(16) atom. Linkers: 4 C[C@@H]1CC(C)(C)NCCN[C@@H](C)CC(C)(C)NCCN1. Metal clusters: 4 [Ni] ,2 [Mo]. The MOF has largest included sphere 4.58 A, density 1.16 g/cm3, surface area 4950.45 m2/g, accessible volume 0.41 cm3/g