NiH(C2N3)3 crystallizes in the monoclinic C2/c space group. Ni(1) is bonded in a rectangular see-saw-like geometry to one N(5), one N(7), one N(8), and one N(9) atom. The Ni(1)-N(5) bond length is 2.03 Å. The Ni(1)-N(7) bond length is 2.04 Å. The Ni(1)-N(8) bond length is 2.21 Å. The Ni(1)-N(9) bond length is 2.07 Å. There are six 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 N(4) atom. The C(1)-N(1) bond length is 1.36 Å. The C(1)-N(2) bond length is 1.35 Å. The C(1)-N(4) bond length is 1.34 Å. In the second C site, C(2) is bonded in a trigonal planar geometry to one N(1), one N(3), and one N(6) atom. The C(2)-N(1) bond length is 1.36 Å. The C(2)-N(3) bond length is 1.28 Å. The C(2)-N(6) bond length is 1.34 Å. In the third C site, C(3) is bonded in a trigonal planar geometry to one N(2), one N(3), and one N(8) atom. The C(3)-N(2) bond length is 1.32 Å. The C(3)-N(3) bond length is 1.31 Å. The C(3)-N(8) bond length is 1.35 Å. In the fourth C site, C(4) is bonded in a linear geometry to one N(4) and one N(5) atom. The C(4)-N(4) bond length is 1.31 Å. The C(4)-N(5) bond length is 1.16 Å. In the fifth C site, C(5) is bonded in a linear geometry to one N(6) and one N(7) atom. The C(5)-N(6) bond length is 1.32 Å. The C(5)-N(7) bond length is 1.15 Å. In the sixth C site, C(6) is bonded in a linear geometry to one N(8) and one N(9) atom. The C(6)-N(8) bond length is 1.32 Å. The C(6)-N(9) bond length is 1.14 Å. There are nine inequivalent N sites. In the first N site, N(1) is bonded in a trigonal planar geometry to one C(1), one C(2), and one H(1) atom. The N(1)-H(1) bond length is 0.86 Å. In the second N site, N(2) is bonded in a bent 120 degrees geometry to one C(1) and one C(3) atom. In the third N site, N(3) is bonded in a bent 120 degrees geometry to one C(2) and one C(3) atom. In the fourth N site, N(4) is bonded in a bent 120 degrees geometry to one C(1) and one C(4) atom. In the fifth N site, N(5) is bonded in a distorted bent 150 degrees geometry to one Ni(1) and one C(4) atom. In the sixth N site, N(6) is bonded in a bent 120 degrees geometry to one C(2) and one C(5) atom. In the seventh N site, N(7) is bonded in a distorted single-bond geometry to one Ni(1) and one C(5) atom. In the eighth N site, N(8) is bonded in a distorted trigonal planar geometry to one Ni(1), one C(3), and one C(6) atom. In the ninth N site, N(9) is bonded in a bent 150 degrees geometry to one Ni(1) and one C(6) atom. H(1) is bonded in a single-bond geometry to one N(1) atom. Linkers: 4 N#C[N]C1=[N]=[C](=[N]=C(N1)[N]C#N)[N]C#N. Metal clusters: 4 [Ni]. The MOF has largest included sphere 5.52 A, density 1.58 g/cm3, surface area 3454.51 m2/g, accessible volume 0.29 cm3/g