Ni4C48H27(N4O)3 is Copper structured and crystallizes in the cubic Fm-3m space group. The structure is zero-dimensional and consists of four Ni4C48H27(N4O)3 clusters. Ni(1) is bonded to three equivalent N(1) and three equivalent O(1) atoms to form a mixture of edge and corner-sharing NiN3O3 octahedra. The corner-sharing octahedral tilt angles are 40°. All Ni(1)-N(1) bond lengths are 1.94 Å. All Ni(1)-O(1) bond lengths are 2.07 Å. There are six inequivalent C sites. In the first C site, C(5) is bonded in a single-bond geometry to one C(1) and one H(2) atom. The C(5)-C(1) bond length is 1.39 Å. The C(5)-H(2) bond length is 0.95 Å. In the second C site, C(6) is bonded in a distorted bent 120 degrees geometry to one C(4), one N(1), and one H(3) atom. The C(6)-C(4) bond length is 1.36 Å. The C(6)-N(1) bond length is 1.36 Å. The C(6)-H(3) bond length is 0.95 Å. In the third C site, C(1) is bonded in a trigonal planar geometry to one C(2) and two equivalent C(5) atoms. The C(1)-C(2) bond length is 1.50 Å. In the fourth C site, C(2) is bonded in a linear geometry to one C(1) and one C(3) atom. The C(2)-C(3) bond length is 1.24 Å. In the fifth C site, C(3) is bonded in a linear geometry to one C(2) and one C(4) atom. The C(3)-C(4) bond length is 1.50 Å. In the sixth C site, C(4) is bonded in a trigonal planar geometry to one C(3) and two equivalent C(6) atoms. N(1) is bonded in a distorted trigonal planar geometry to one Ni(1), one C(6), and one N(1) atom. The N(1)-N(1) bond length is 1.36 Å. There are three inequivalent H sites. In the first H site, H(1) is bonded in a single-bond geometry to one O(1) atom. The H(1)-O(1) bond length is 0.95 Å. In the second H site, H(2) is bonded in a single-bond geometry to one C(5) atom. In the third H site, H(3) is bonded in a single-bond geometry to one C(6) atom. O(1) is bonded in a distorted single-bond geometry to four equivalent Ni(1) and one H(1) atom. Linkers: 5 C(#Cc1ccc(C#CC2=C[N]N=C2)cc1)[C]1C=NN=C1 ,1 C(#Cc1ccc(C#CC2=C[N]N=C2)cc1)C1=C[N]N=C1. Metal clusters: 1 O[Ni@@]12[N][N][Ni]3[N][N][Ni]4[N][N][Ni@@](O)([N][N]1)[N][N][Ni@@]1(O)[N][N][Ni@](O)([N][N][Ni]([N][N]3)[N][N][Ni](O)(O)([N][N]4)[N][N]1)[N][N]2. The MOF has largest included sphere 19.69 A, density 0.41 g/cm3, surface area 4202.02 m2/g, accessible volume 2.00 cm3/g