Ni2H6(C5N2)3 crystallizes in the cubic Fm-3m space group. Ni(1) is bonded in a 3-coordinate geometry to three equivalent N(1) atoms. All Ni(1)-N(1) bond lengths are 2.07 Å. There are four inequivalent C sites. In the first C site, C(2) is bonded in a linear geometry to one C(1) and one C(3) atom. The C(2)-C(1) bond length is 1.25 Å. The C(2)-C(3) bond length is 1.39 Å. In the second C site, C(1) is bonded in a linear geometry to one C(1) and one C(2) atom. The C(1)-C(1) bond length is 1.39 Å. In the third C site, C(3) is bonded in a trigonal planar geometry to one C(2) and two equivalent C(4) atoms. Both C(3)-C(4) bond lengths are 1.36 Å. In the fourth C site, C(4) is bonded in a distorted bent 120 degrees geometry to one C(3), one N(1), and one H(1) atom. The C(4)-N(1) bond length is 1.36 Å. The C(4)-H(1) bond length is 0.95 Å. N(1) is bonded in a distorted bent 150 degrees geometry to one Ni(1) and one C(4) atom. H(1) is bonded in a single-bond geometry to one C(4) atom. Linkers: 2 C(C#CC1=C[N]N=C1)#C[C]1C=NN=C1 ,3 C(C#CC1=C[N]N=C1)#CC1=CN=N[CH]1 ,1 C(C#CC1=CN=N[CH]1)#CC1=CN=N[CH]1. Metal clusters: 1 [N]1[N][Ni]2345[N][N][Ni]2678[N][N][Ni]629%10[N][N][Ni]1326[N][N][Ni]6123[N][N][Ni]416([N][N]5)[N][N][Ni]761([N][N]8)[N][N][Ni]921([N][N]%10)[N][N]3. The MOF has largest included sphere 15.37 A, density 0.55 g/cm3, surface area 4260.17 m2/g, accessible volume 1.41 cm3/g