ZnH4(CN5)2 crystallizes in the monoclinic Cc space group. Zn(1) is bonded in a tetrahedral geometry to one N(10), one N(2), one N(5), and one N(7) atom. The Zn(1)-N(10) bond length is 2.00 Å. The Zn(1)-N(2) bond length is 1.99 Å. The Zn(1)-N(5) bond length is 1.99 Å. The Zn(1)-N(7) bond length is 2.00 Å. There are two 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(5) atom. The C(1)-N(1) bond length is 1.33 Å. The C(1)-N(2) bond length is 1.36 Å. The C(1)-N(5) bond length is 1.36 Å. In the second C site, C(2) is bonded in a trigonal planar geometry to one N(10), one N(6), and one N(7) atom. The C(2)-N(10) bond length is 1.35 Å. The C(2)-N(6) bond length is 1.35 Å. The C(2)-N(7) bond length is 1.35 Å. There are ten inequivalent N sites. In the first N site, N(3) is bonded in a water-like geometry to one N(2) and one N(4) atom. The N(3)-N(2) bond length is 1.36 Å. The N(3)-N(4) bond length is 1.29 Å. In the second N site, N(4) is bonded in a water-like geometry to one N(3) and one N(5) atom. The N(4)-N(5) bond length is 1.37 Å. In the third N site, N(5) is bonded in a distorted trigonal planar geometry to one Zn(1), one C(1), and one N(4) atom. In the fourth N site, N(6) is bonded in a trigonal planar geometry to one C(2), one H(3), and one H(4) atom. The N(6)-H(3) bond length is 1.02 Å. The N(6)-H(4) bond length is 1.02 Å. In the fifth N site, N(7) is bonded in a 2-coordinate geometry to one Zn(1), one C(2), and one N(8) atom. The N(7)-N(8) bond length is 1.37 Å. In the sixth N site, N(8) is bonded in a water-like geometry to one N(7) and one N(9) atom. The N(8)-N(9) bond length is 1.29 Å. In the seventh N site, N(9) is bonded in a distorted water-like geometry to one N(10) and one N(8) atom. The N(9)-N(10) bond length is 1.37 Å. In the eighth N site, N(10) is bonded in a 3-coordinate geometry to one Zn(1), one C(2), and one N(9) atom. In the ninth N site, N(1) is bonded in a trigonal planar geometry to one C(1), one H(1), and one H(2) atom. The N(1)-H(1) bond length is 1.03 Å. The N(1)-H(2) bond length is 1.03 Å. In the tenth N site, N(2) is bonded in a distorted trigonal planar geometry to one Zn(1), one C(1), and one N(3) atom. There are four inequivalent H sites. In the first H site, H(1) is bonded in a single-bond geometry to one N(1) atom. In the second H site, H(2) is bonded in a single-bond geometry to one N(1) atom. In the third H site, H(3) is bonded in a single-bond geometry to one N(6) atom. In the fourth H site, H(4) is bonded in a single-bond geometry to one N(6) atom. Linkers: 4 NC1=NN=N[N]1. Metal clusters: 2 [Zn]. The MOF has largest included sphere 6.10 A, density 1.13 g/cm3, surface area 3762.98 m2/g, accessible volume 0.51 cm3/g