ZnH2(CN2)5 crystallizes in the monoclinic Cc space group. There are two inequivalent Zn sites. In the first Zn site, Zn(1) is bonded in a trigonal bipyramidal geometry to one N(11), one N(17), one N(4), one N(5), and one N(8) atom. The Zn(1)-N(11) bond length is 2.03 Å. The Zn(1)-N(17) bond length is 2.18 Å. The Zn(1)-N(4) bond length is 2.09 Å. The Zn(1)-N(5) bond length is 2.18 Å. The Zn(1)-N(8) bond length is 2.03 Å. In the second Zn site, Zn(2) is bonded in a trigonal bipyramidal geometry to one N(1), one N(14), one N(15), one N(18), and one N(7) atom. The Zn(2)-N(1) bond length is 2.05 Å. The Zn(2)-N(14) bond length is 2.08 Å. The Zn(2)-N(15) bond length is 2.21 Å. The Zn(2)-N(18) bond length is 2.02 Å. The Zn(2)-N(7) bond length is 2.17 Å. There are ten inequivalent C sites. In the first C site, C(1) is bonded in a distorted trigonal planar geometry to one C(2), one N(1), and one N(4) atom. The C(1)-C(2) bond length is 1.44 Å. The C(1)-N(1) bond length is 1.34 Å. The C(1)-N(4) bond length is 1.35 Å. In the second C site, C(2) is bonded in a distorted single-bond geometry to one C(1), one C(4), and one N(5) atom. The C(2)-C(4) bond length is 1.39 Å. The C(2)-N(5) bond length is 1.38 Å. In the third C site, C(3) is bonded in a trigonal planar geometry to one N(5), one N(6), and one H(3) atom. The C(3)-N(5) bond length is 1.33 Å. The C(3)-N(6) bond length is 1.35 Å. The C(3)-H(3) bond length is 1.08 Å. In the fourth C site, C(4) is bonded in a distorted single-bond geometry to one C(2), one C(5), and one N(6) atom. The C(4)-C(5) bond length is 1.44 Å. The C(4)-N(6) bond length is 1.38 Å. In the fifth C site, C(5) is bonded in a distorted trigonal planar geometry to one C(4), one N(10), and one N(7) atom. The C(5)-N(10) bond length is 1.35 Å. The C(5)-N(7) bond length is 1.35 Å. In the sixth C site, C(6) is bonded in a distorted trigonal planar geometry to one C(7), one N(11), and one N(14) atom. The C(6)-C(7) bond length is 1.44 Å. The C(6)-N(11) bond length is 1.34 Å. The C(6)-N(14) bond length is 1.35 Å. In the seventh C site, C(7) is bonded in a distorted single-bond geometry to one C(6), one C(9), and one N(15) atom. The C(7)-C(9) bond length is 1.39 Å. The C(7)-N(15) bond length is 1.39 Å. In the eighth C site, C(8) is bonded in a trigonal planar geometry to one N(15), one N(16), and one H(4) atom. The C(8)-N(15) bond length is 1.33 Å. The C(8)-N(16) bond length is 1.35 Å. The C(8)-H(4) bond length is 1.08 Å. In the ninth C site, C(9) is bonded in a distorted single-bond geometry to one C(10), one C(7), and one N(16) atom. The C(9)-C(10) bond length is 1.44 Å. The C(9)-N(16) bond length is 1.38 Å. In the tenth C site, C(10) is bonded in a distorted water-like geometry to one C(9), one N(17), and one N(20) atom. The C(10)-N(17) bond length is 1.35 Å. The C(10)-N(20) bond length is 1.35 Å. There are twenty inequivalent N sites. In the first N site, N(1) is bonded in a distorted trigonal planar geometry to one Zn(2), one C(1), and one N(2) atom. The N(1)-N(2) bond length is 1.36 Å. In the second N site, N(2) is bonded in a 3-coordinate geometry to one N(1), one N(3), and one H(1) atom. The N(2)-N(3) bond length is 1.31 Å. The N(2)-H(1) bond length is 1.80 Å. In the third N site, N(3) is bonded in a water-like geometry to one N(2) and one N(4) atom. The N(3)-N(4) bond length is 1.34 Å. In the fourth N site, N(4) is bonded in a 3-coordinate geometry to one Zn(1), one C(1), and one N(3) atom. In the fifth N site, N(5) is bonded in a distorted trigonal non-coplanar geometry to one Zn(1), one C(2), and one C(3) atom. In the sixth N site, N(6) is bonded in a trigonal planar geometry to one C(3), one C(4), and one H(1) atom. The N(6)-H(1) bond length is 1.04 Å. In the seventh N site, N(7) is bonded in a distorted trigonal planar geometry to one Zn(2), one C(5), and one N(8) atom. The N(7)-N(8) bond length is 1.35 Å. In the eighth N site, N(8) is bonded in a distorted trigonal planar geometry to one Zn(1), one N(7), and one N(9) atom. The N(8)-N(9) bond length is 1.33 Å. In the ninth N site, N(9) is bonded in a water-like geometry to one N(10) and one N(8) atom. The N(9)-N(10) bond length is 1.33 Å. In the tenth N site, N(10) is bonded in a distorted single-bond geometry to one C(5) and one N(9) atom. In the eleventh N site, N(11) is bonded in a 3-coordinate geometry to one Zn(1), one C(6), 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 water-like geometry to one N(11) and one N(13) atom. The N(12)-N(13) bond length is 1.31 Å. In the thirteenth N site, N(13) is bonded in a water-like geometry to one N(12) and one N(14) atom. The N(13)-N(14) bond length is 1.35 Å. In the fourteenth N site, N(14) is bonded in a 3-coordinate geometry to one Zn(2), one C(6), and one N(13) atom. In the fifteenth N site, N(15) is bonded in a distorted trigonal non-coplanar geometry to one Zn(2), one C(7), and one C(8) atom. In the sixteenth N site, N(16) is bonded in a distorted trigonal planar geometry to one C(8), one C(9), and one H(2) atom. The N(16)-H(2) bond length is 1.02 Å. In the seventeenth N site, N(17) is bonded in a distorted trigonal planar geometry to one Zn(1), one C(10), and one N(18) atom. The N(17)-N(18) bond length is 1.34 Å. In the eighteenth N site, N(18) is bonded in a distorted trigonal planar geometry to one Zn(2), one N(17), and one N(19) atom. The N(18)-N(19) bond length is 1.33 Å. In the nineteenth N site, N(19) is bonded in a water-like geometry to one N(18) and one N(20) atom. The N(19)-N(20) bond length is 1.33 Å. In the twentieth N site, N(20) is bonded in a distorted single-bond geometry to one C(10) and one N(19) atom. There are four inequivalent H sites. In the first H site, H(1) is bonded in a single-bond geometry to one N(2) and one N(6) atom. In the second H site, H(2) is bonded in a single-bond geometry to one N(16) 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(8) atom. Linkers: 4 c1nc(C2=NN=N[N]2)c(C2=NN=N[N]2)[nH]1. Metal clusters: 2 [N]1[N][Zn][N][N][Zn]1. The MOF has largest included sphere 5.14 A, density 1.58 g/cm3, surface area 3407.52 m2/g, accessible volume 0.29 cm3/g