NiH6(C5N2)2 crystallizes in the cubic Pm-3m space group. Ni(1) is bonded in a distorted square co-planar geometry to four equivalent N(1) atoms. All Ni(1)-N(1) bond lengths are 2.02 Å. There are four inequivalent C sites. In the first C site, C(2) is bonded in a trigonal planar geometry to one C(3) and two equivalent C(4) atoms. The C(2)-C(3) bond length is 1.45 Å. Both C(2)-C(4) bond lengths are 1.38 Å. In the second C site, C(3) is bonded in a trigonal planar geometry to one C(2) and two equivalent C(1) atoms. Both C(3)-C(1) bond lengths are 1.36 Å. In the third C site, C(1) is bonded in a distorted bent 120 degrees geometry to one C(3), one N(1), and one H(1) atom. The C(1)-N(1) bond length is 1.36 Å. The C(1)-H(1) bond length is 0.95 Å. In the fourth C site, C(4) is bonded in a trigonal planar geometry to two equivalent C(2) and one H(2) atom. The C(4)-H(2) bond length is 0.95 Å. N(1) is bonded in a 3-coordinate geometry to one Ni(1), one C(1), and one N(1) atom. The N(1)-N(1) bond length is 1.36 Å. There are two 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(4) atom. Linkers: 4 [CH]1N=NC=C1c1cc(C2=C[N]N=C2)cc(C2=C[N]N=C2)c1 ,4 [CH]1N=NC=C1c1cc([C]2C=NN=C2)cc(C2=C[N]N=C2)c1. Metal clusters: 3 N1=N[Ni]23=NN=[Ni]14N=N[Ni]1(=NN=[Ni](N=N2)(N=N1)N=N3)N=N4. The MOF has largest included sphere 14.59 A, density 0.75 g/cm3, surface area 3716.89 m2/g, accessible volume 0.86 cm3/g