NiH6(C4N3)2 crystallizes in the cubic Ia-3d space group. Ni(1) is bonded in a square pyramidal geometry to one N(1), one N(2), one N(3), one N(4), and one N(5) atom. The Ni(1)-N(1) bond length is 2.01 Å. The Ni(1)-N(2) bond length is 2.02 Å. The Ni(1)-N(3) bond length is 2.03 Å. The Ni(1)-N(4) bond length is 1.99 Å. The Ni(1)-N(5) bond length is 2.07 Å. There are eight inequivalent C sites. In the first 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 1.34 Å. The C(1)-N(2) bond length is 1.37 Å. The C(1)-H(1) bond length is 0.95 Å. In the second C site, C(2) is bonded in a trigonal planar geometry to one N(3), one N(4), and one H(2) atom. The C(2)-N(3) bond length is 1.40 Å. The C(2)-N(4) bond length is 1.32 Å. The C(2)-H(2) bond length is 0.95 Å. In the third C site, C(3) is bonded in a distorted single-bond geometry to one C(8) and one N(1) atom. The C(3)-C(8) bond length is 1.40 Å. The C(3)-N(1) bond length is 1.42 Å. In the fourth C site, C(4) is bonded in a distorted bent 120 degrees geometry to one C(6), one N(3), and one H(3) atom. The C(4)-C(6) bond length is 1.40 Å. The C(4)-N(3) bond length is 1.39 Å. The C(4)-H(3) bond length is 0.95 Å. In the fifth C site, C(5) is bonded in a distorted bent 120 degrees geometry to one N(2) and one H(4) atom. The C(5)-N(2) bond length is 1.37 Å. The C(5)-H(4) bond length is 0.95 Å. In the sixth C site, C(6) is bonded in a 3-coordinate geometry to one C(4), one C(7), and one N(4) atom. The C(6)-C(7) bond length is 1.40 Å. The C(6)-N(4) bond length is 1.41 Å. In the seventh C site, C(7) is bonded in a distorted trigonal planar geometry to one C(6), one N(6), and one H(5) atom. The C(7)-N(6) bond length is 1.37 Å. The C(7)-H(5) bond length is 0.95 Å. In the eighth C site, C(8) is bonded in a distorted trigonal planar geometry to one C(3), one N(5), and one H(6) atom. The C(8)-N(5) bond length is 1.39 Å. The C(8)-H(6) bond length is 0.94 Å. There are six inequivalent N sites. In the first N site, N(1) is bonded in a distorted trigonal planar geometry to one Ni(1), one C(1), and one C(3) atom. In the second N site, N(2) is bonded in a distorted trigonal planar geometry to one Ni(1), one C(1), and one C(5) atom. In the third N site, N(3) is bonded in a distorted trigonal planar geometry to one Ni(1), one C(2), and one C(4) atom. In the fourth N site, N(4) is bonded in a distorted trigonal planar geometry to one Ni(1), one C(2), and one C(6) atom. In the fifth N site, N(5) is bonded in a distorted bent 120 degrees geometry to one Ni(1) and one C(8) atom. In the sixth N site, N(6) is bonded in a single-bond geometry to one C(7) atom. There are six 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(4) 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(7) atom. In the sixth H site, H(6) is bonded in a single-bond geometry to one C(8) atom. Linkers: 47 [CH]([N][N]/C=C1/C=NC=N1)C1=CN=C[N]1 ,1 [CH]([N][N]/C=C1/C=NC=N1)[C]1C=NC=N1. Metal clusters: 48 [Ni]. The MOF has largest included sphere 8.18 A, density 1.01 g/cm3, surface area 3977.94 m2/g, accessible volume 0.67 cm3/g