ZnH4(CN2)4 crystallizes in the orthorhombic Pbca space group. Zn(1) is bonded in a trigonal bipyramidal geometry to one N(1), one N(2), one N(3), one N(5), and one N(6) atom. The Zn(1)-N(1) bond length is 2.02 Å. The Zn(1)-N(2) bond length is 2.01 Å. The Zn(1)-N(3) bond length is 2.37 Å. The Zn(1)-N(5) bond length is 2.01 Å. The Zn(1)-N(6) bond length is 2.20 Å. There are four inequivalent C sites. In the first C site, C(4) is bonded in a distorted trigonal planar geometry to one C(1), one N(5), and one N(6) atom. The C(4)-C(1) bond length is 1.49 Å. The C(4)-N(5) bond length is 1.35 Å. The C(4)-N(6) bond length is 1.34 Å. In the second C site, C(1) is bonded in a distorted water-like geometry to one C(4), one H(1), and one H(2) atom. The C(1)-H(1) bond length is 1.10 Å. The C(1)-H(2) bond length is 1.10 Å. In the third C site, C(2) is bonded in a distorted trigonal planar geometry to one C(3), one N(1), and one N(2) atom. The C(2)-C(3) bond length is 1.49 Å. The C(2)-N(1) bond length is 1.35 Å. The C(2)-N(2) bond length is 1.34 Å. In the fourth C site, C(3) is bonded in a distorted water-like geometry to one C(2), one H(3), and one H(4) atom. The C(3)-H(3) bond length is 1.10 Å. The C(3)-H(4) bond length is 1.10 Å. There are eight inequivalent N sites. In the first N site, N(4) is bonded in a water-like geometry to one N(1) and one N(3) atom. The N(4)-N(1) bond length is 1.35 Å. The N(4)-N(3) bond length is 1.30 Å. In the second N site, N(8) is bonded in a water-like geometry to one N(6) and one N(7) atom. The N(8)-N(6) bond length is 1.36 Å. The N(8)-N(7) bond length is 1.30 Å. In the third N site, N(1) is bonded in a 3-coordinate geometry to one Zn(1), one C(2), and one N(4) atom. In the fourth N site, N(5) is bonded in a 3-coordinate geometry to one Zn(1), one C(4), and one N(7) atom. The N(5)-N(7) bond length is 1.36 Å. In the fifth N site, N(2) is bonded in a distorted trigonal planar geometry to one Zn(1), one C(2), and one N(3) atom. The N(2)-N(3) bond length is 1.36 Å. In the sixth N site, N(6) is bonded in a 3-coordinate geometry to one Zn(1), one C(4), and one N(8) atom. In the seventh N site, N(3) is bonded in a trigonal non-coplanar geometry to one Zn(1), one N(2), and one N(4) atom. In the eighth N site, N(7) is bonded in a water-like geometry to one N(5) and one N(8) atom. There are four inequivalent H sites. In the first H site, H(4) is bonded in a single-bond geometry to one C(3) atom. In the second H site, H(1) is bonded in a single-bond geometry to one C(1) atom. In the third H site, H(2) is bonded in a single-bond geometry to one C(1) atom. In the fourth H site, H(3) is bonded in a single-bond geometry to one C(3) atom. Linkers: 8 C(CC1=NN=N[N]1)C1=NN=N[N]1. Metal clusters: 4 [N]1[N][Zn][N][N][Zn]1. The MOF has largest included sphere 2.19 A, density 2.16 g/cm3, surface area 3084.31 m2/g, accessible volume 0.12 cm3/g