ZnH4(CN2)4 crystallizes in the monoclinic Pc space group. There are two inequivalent Zn sites. In the first Zn site, Zn(1) is bonded in a tetrahedral geometry to one N(1), one N(3), one N(5), and one N(9) atom. The Zn(1)-N(1) bond length is 1.99 Å. The Zn(1)-N(3) bond length is 2.01 Å. The Zn(1)-N(5) bond length is 1.99 Å. The Zn(1)-N(9) bond length is 2.06 Å. In the second Zn site, Zn(2) is bonded in a tetrahedral geometry to one N(12), one N(13), one N(16), and one N(8) atom. The Zn(2)-N(12) bond length is 2.00 Å. The Zn(2)-N(13) bond length is 2.01 Å. The Zn(2)-N(16) bond length is 2.01 Å. The Zn(2)-N(8) bond length is 1.98 Å. There are eight inequivalent C sites. In the first C site, C(1) is bonded in a distorted trigonal planar geometry to one C(2), one N(3), and one N(4) atom. The C(1)-C(2) bond length is 1.48 Å. The C(1)-N(3) bond length is 1.36 Å. The C(1)-N(4) bond length is 1.34 Å. In the second C site, C(2) is bonded in a distorted water-like geometry to one C(1), one H(1), and one H(2) atom. The C(2)-H(1) bond length is 1.10 Å. The C(2)-H(2) bond length is 1.09 Å. In the third C site, C(3) is bonded in a distorted water-like geometry to one C(4), one H(3), and one H(4) atom. The C(3)-C(4) bond length is 1.49 Å. The C(3)-H(3) bond length is 1.10 Å. The C(3)-H(4) bond length is 1.10 Å. In the fourth C site, C(4) is bonded in a distorted trigonal planar geometry to one C(3), one N(5), and one N(8) atom. The C(4)-N(5) bond length is 1.35 Å. The C(4)-N(8) bond length is 1.34 Å. In the fifth C site, C(5) is bonded in a distorted trigonal planar geometry to one C(6), one N(12), and one N(9) atom. The C(5)-C(6) bond length is 1.49 Å. The C(5)-N(12) bond length is 1.34 Å. The C(5)-N(9) bond length is 1.35 Å. In the sixth C site, C(6) is bonded in a distorted water-like geometry to one C(5), one H(5), and one H(6) atom. The C(6)-H(5) bond length is 1.10 Å. The C(6)-H(6) bond length is 1.10 Å. In the seventh C site, C(7) is bonded in a water-like geometry to one C(8), one H(7), and one H(8) atom. The C(7)-C(8) bond length is 1.50 Å. The C(7)-H(7) bond length is 1.10 Å. The C(7)-H(8) bond length is 1.10 Å. In the eighth C site, C(8) is bonded in a distorted trigonal planar geometry to one C(7), one N(13), and one N(16) atom. The C(8)-N(13) bond length is 1.35 Å. The C(8)-N(16) bond length is 1.34 Å. There are sixteen inequivalent N sites. In the first N site, N(1) is bonded in a trigonal planar geometry to one Zn(1), one N(2), and one N(4) atom. The N(1)-N(2) bond length is 1.31 Å. The N(1)-N(4) bond length is 1.34 Å. In the second N site, N(2) is bonded in a water-like geometry to one N(1) and one N(3) atom. The N(2)-N(3) bond length is 1.34 Å. In the third N site, N(3) is bonded in a 3-coordinate geometry to one Zn(1), one C(1), and one N(2) atom. In the fourth N site, N(4) is bonded in a distorted water-like geometry to one C(1) and one N(1) atom. In the fifth N site, N(5) is bonded in a distorted trigonal planar geometry to one Zn(1), one C(4), and one N(6) atom. The N(5)-N(6) bond length is 1.36 Å. In the sixth N site, N(6) is bonded in a water-like geometry to one N(5) and one N(7) atom. The N(6)-N(7) bond length is 1.30 Å. In the seventh N site, N(7) is bonded in a water-like geometry to one N(6) and one N(8) atom. The N(7)-N(8) bond length is 1.36 Å. In the eighth N site, N(8) is bonded in a 3-coordinate geometry to one Zn(2), one C(4), and one N(7) atom. In the ninth N site, N(9) is bonded in a 3-coordinate geometry to one Zn(1), one C(5), and one N(10) atom. The N(9)-N(10) bond length is 1.36 Å. In the tenth N site, N(10) is bonded in a water-like geometry to one N(11) and one N(9) atom. The N(10)-N(11) bond length is 1.30 Å. In the eleventh N site, N(11) is bonded in a water-like geometry to one N(10) and one N(12) atom. The N(11)-N(12) bond length is 1.36 Å. In the twelfth N site, N(12) is bonded in a distorted trigonal planar geometry to one Zn(2), one C(5), and one N(11) atom. In the thirteenth N site, N(13) is bonded in a 3-coordinate geometry to one Zn(2), one C(8), and one N(14) atom. The N(13)-N(14) bond length is 1.36 Å. In the fourteenth N site, N(14) is bonded in a water-like geometry to one N(13) and one N(15) atom. The N(14)-N(15) bond length is 1.29 Å. In the fifteenth N site, N(15) is bonded in a water-like geometry to one N(14) and one N(16) atom. The N(15)-N(16) bond length is 1.36 Å. In the sixteenth N site, N(16) is bonded in a 3-coordinate geometry to one Zn(2), one C(8), and one N(15) atom. There are eight inequivalent H sites. In the first H site, H(1) is bonded in a single-bond geometry to one C(2) 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(3) atom. In the fourth H site, H(4) is bonded in a single-bond geometry to one C(3) atom. In the fifth H site, H(5) is bonded in a single-bond geometry to one C(6) atom. In the sixth H site, H(6) is bonded in a single-bond geometry to one C(6) atom. In the seventh H site, H(7) is bonded in a single-bond geometry to one C(7) atom. In the eighth H site, H(8) is bonded in a single-bond geometry to one C(7) atom. Linkers: 4 C(CC1=NN=N[N]1)C1=NN=N[N]1. Metal clusters: 4 [Zn]. The MOF has largest included sphere 3.08 A, density 2.00 g/cm3, surface area 3572.28 m2/g, accessible volume 0.13 cm3/g