Mo6Ni2C48N16H40O19 crystallizes in the tetragonal I4/m space group. There are five inequivalent Mo sites. In the first Mo site, Mo(1) is bonded in a 6-coordinate geometry to one O(1), one O(3), two equivalent O(2), and two equivalent O(4) atoms. The Mo(1)-O(1) bond length is 1.74 Å. The Mo(1)-O(3) bond length is 2.35 Å. There is one shorter (1.81 Å) and one longer (2.18 Å) Mo(1)-O(2) bond length. Both Mo(1)-O(4) bond lengths are 1.90 Å. In the second Mo site, Mo(1) is bonded in a 6-coordinate geometry to one O(1), one O(3), two equivalent O(2), and two equivalent O(4) atoms. The Mo(1)-O(1) bond length is 1.74 Å. The Mo(1)-O(3) bond length is 2.35 Å. There is one shorter (1.81 Å) and one longer (2.18 Å) Mo(1)-O(2) bond length. Both Mo(1)-O(4) bond lengths are 1.90 Å. In the third Mo site, Mo(1) is bonded in a 6-coordinate geometry to one O(1), one O(3), two equivalent O(2), and two equivalent O(4) atoms. The Mo(1)-O(1) bond length is 1.74 Å. The Mo(1)-O(3) bond length is 2.35 Å. There is one shorter (1.81 Å) and one longer (2.18 Å) Mo(1)-O(2) bond length. Both Mo(1)-O(4) bond lengths are 1.90 Å. In the fourth Mo site, Mo(2) is bonded in a 6-coordinate geometry to one O(3), one O(5), and four equivalent O(4) atoms. The Mo(2)-O(3) bond length is 2.36 Å. The Mo(2)-O(5) bond length is 1.71 Å. All Mo(2)-O(4) bond lengths are 1.99 Å. In the fifth Mo site, Mo(1) is bonded in a 6-coordinate geometry to one O(1), one O(3), two equivalent O(2), and two equivalent O(4) atoms. The Mo(1)-O(1) bond length is 1.74 Å. The Mo(1)-O(3) bond length is 2.35 Å. There is one shorter (1.81 Å) and one longer (2.18 Å) Mo(1)-O(2) bond length. Both Mo(1)-O(4) bond lengths are 1.90 Å. Ni(1) is bonded in an octahedral geometry to four equivalent N(1) and two equivalent O(1) atoms. All Ni(1)-N(1) bond lengths are 2.06 Å. Both Ni(1)-O(1) bond lengths are 2.06 Å. There are six inequivalent C sites. In the first C site, C(5) is bonded in a distorted single-bond geometry to one C(4), one C(6), and one H(4) atom. The C(5)-C(4) bond length is 1.40 Å. The C(5)-C(6) bond length is 1.39 Å. The C(5)-H(4) bond length is 1.09 Å. In the second C site, C(6) is bonded in a distorted trigonal planar geometry to one C(4), one C(5), and one H(5) atom. The C(6)-C(4) bond length is 1.40 Å. The C(6)-H(5) bond length is 1.09 Å. In the third C site, C(1) is bonded in a trigonal planar geometry to one N(1), one N(2), and one H(1) atom. The C(1)-N(1) bond length is 1.32 Å. The C(1)-N(2) bond length is 1.37 Å. The C(1)-H(1) bond length is 1.09 Å. In the fourth C site, C(2) is bonded in a distorted bent 120 degrees geometry to one N(1) and one H(2) atom. The C(2)-N(1) bond length is 1.38 Å. The C(2)-H(2) bond length is 1.08 Å. In the fifth C site, C(3) is bonded in a distorted bent 120 degrees geometry to one N(2) and one H(3) atom. The C(3)-N(2) bond length is 1.39 Å. The C(3)-H(3) bond length is 1.08 Å. In the sixth C site, C(4) is bonded in a distorted trigonal planar geometry to one C(5), one C(6), and one N(2) atom. The C(4)-N(2) bond length is 1.42 Å. There are two 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(2) atom. In the second N site, N(2) is bonded in a trigonal planar geometry to one C(1), one C(3), and one C(4) atom. There are five inequivalent H sites. In the first H site, H(1) is bonded in a single-bond geometry to one C(1) 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 C(3) atom. In the fourth H site, H(4) is bonded in a single-bond geometry to one C(5) atom. In the fifth H site, H(5) is bonded in a single-bond geometry to one C(6) atom. There are five inequivalent O sites. In the first O site, O(1) is bonded in a linear geometry to one Mo(1) and one Ni(1) atom. In the second O site, O(2) is bonded in a bent 120 degrees geometry to two Mo(1,1) atoms. In the third O site, O(3) is bonded in an octahedral geometry to two equivalent Mo(2) and four Mo(1,1) atoms. In the fourth O site, O(4) is bonded in a bent 120 degrees geometry to one Mo(1) and one Mo(2) atom. In the fifth O site, O(5) is bonded in a single-bond geometry to one Mo(2) atom. Linkers: 4 c1cn(-c2ccc(-n3ccnc3)cc2)cn1. Metal clusters: 2 [Ni] ,6 [Mo]. The MOF has largest included sphere 4.83 A, density 1.99 g/cm3, surface area 3170.62 m2/g, accessible volume 0.13 cm3/g