ZnH4(CN)8 is Indium-like structured and crystallizes in the triclinic P-1 space group. The structure is zero-dimensional and consists of one ZnH4(CN)8 cluster. There are two inequivalent Zn sites. In the first Zn site, Zn(1) is bonded in a distorted T-shaped geometry to one N(3), one N(5), and one N(7) atom. The Zn(1)-N(3) bond length is 2.14 Å. The Zn(1)-N(5) bond length is 2.14 Å. The Zn(1)-N(7) bond length is 2.17 Å. In the second Zn site, Zn(2) is bonded in an octahedral geometry to two equivalent N(6), two equivalent N(8), and two equivalent N(9) atoms. Both Zn(2)-N(6) bond lengths are 2.11 Å. Both Zn(2)-N(8) bond lengths are 2.18 Å. Both Zn(2)-N(9) bond lengths are 2.19 Å. There are twelve inequivalent C sites. In the first C site, C(1) is bonded in a 2-coordinate geometry to one C(10), one N(10), and one N(2) atom. The C(1)-C(10) bond length is 1.48 Å. The C(1)-N(10) bond length is 1.34 Å. The C(1)-N(2) bond length is 1.35 Å. In the second C site, C(2) is bonded in a distorted trigonal planar geometry to one C(4), one N(11), and one N(4) atom. The C(2)-C(4) bond length is 1.47 Å. The C(2)-N(11) bond length is 1.34 Å. The C(2)-N(4) bond length is 1.33 Å. In the third C site, C(3) is bonded in a distorted trigonal planar geometry to one C(5), one N(1), and one N(12) atom. The C(3)-C(5) bond length is 1.48 Å. The C(3)-N(1) bond length is 1.34 Å. The C(3)-N(12) bond length is 1.34 Å. In the fourth C site, C(4) is bonded in a trigonal planar geometry to one C(2), one C(7), and one C(9) atom. The C(4)-C(7) bond length is 1.38 Å. The C(4)-C(9) bond length is 1.37 Å. In the fifth C site, C(5) is bonded in a trigonal planar geometry to one C(11), one C(3), and one C(8) atom. The C(5)-C(11) bond length is 1.38 Å. The C(5)-C(8) bond length is 1.38 Å. In the sixth C site, C(6) is bonded in a distorted single-bond geometry to one C(10) and one H(1) atom. The C(6)-C(10) bond length is 1.36 Å. The C(6)-H(1) bond length is 0.93 Å. In the seventh C site, C(7) is bonded in a distorted single-bond geometry to one C(4) and one H(2) atom. The C(7)-H(2) bond length is 0.93 Å. In the eighth C site, C(8) is bonded in a distorted single-bond geometry to one C(5) and one H(3) atom. The C(8)-H(3) bond length is 0.93 Å. In the ninth C site, C(9) is bonded in a distorted single-bond geometry to one C(4) and one H(4) atom. The C(9)-H(4) bond length is 0.93 Å. In the tenth C site, C(10) is bonded in a trigonal planar geometry to one C(1), one C(12), and one C(6) atom. The C(10)-C(12) bond length is 1.34 Å. In the eleventh C site, C(11) is bonded in a distorted single-bond geometry to one C(5) and one H(5) atom. The C(11)-H(5) bond length is 0.93 Å. In the twelfth C site, C(12) is bonded in a single-bond geometry to one C(10) and one H(6) atom. The C(12)-H(6) bond length is 0.93 Å. There are twelve inequivalent N sites. In the first N site, N(1) is bonded in a distorted water-like geometry to one C(3) and one N(5) atom. The N(1)-N(5) bond length is 1.34 Å. In the second N site, N(2) is bonded in a distorted water-like geometry to one C(1) and one N(7) atom. The N(2)-N(7) bond length is 1.32 Å. In the third N site, N(3) is bonded in a distorted trigonal planar geometry to one Zn(1), one N(11), and one N(6) atom. The N(3)-N(11) bond length is 1.34 Å. The N(3)-N(6) bond length is 1.32 Å. In the fourth N site, N(4) is bonded in a water-like geometry to one C(2) and one N(6) atom. The N(4)-N(6) bond length is 1.33 Å. In the fifth N site, N(5) is bonded in a distorted trigonal planar geometry to one Zn(1), one N(1), and one N(9) atom. The N(5)-N(9) bond length is 1.32 Å. In the sixth N site, N(6) is bonded in a distorted trigonal planar geometry to one Zn(2), one N(3), and one N(4) atom. In the seventh N site, N(7) is bonded in a distorted trigonal planar geometry to one Zn(1), one N(2), and one N(8) atom. The N(7)-N(8) bond length is 1.32 Å. In the eighth N site, N(8) is bonded in a distorted trigonal planar geometry to one Zn(2), one N(10), and one N(7) atom. The N(8)-N(10) bond length is 1.33 Å. In the ninth N site, N(9) is bonded in a distorted trigonal planar geometry to one Zn(2), one N(12), and one N(5) atom. The N(9)-N(12) bond length is 1.34 Å. In the tenth N site, N(10) is bonded in a water-like geometry to one C(1) and one N(8) atom. In the eleventh N site, N(11) is bonded in a distorted single-bond geometry to one C(2) and one N(3) atom. In the twelfth N site, N(12) is bonded in a water-like geometry to one C(3) and one N(9) atom. There are six inequivalent H sites. In the first H site, H(1) is bonded in a single-bond geometry to one C(6) atom. In the second H site, H(2) is bonded in a single-bond geometry to one C(7) atom. In the third H site, H(3) is bonded in a single-bond geometry to one C(8) atom. In the fourth H site, H(4) is bonded in a single-bond geometry to one C(9) atom. In the fifth H site, H(5) is bonded in a single-bond geometry to one C(11) atom. In the sixth H site, H(6) is bonded in a single-bond geometry to one C(12) atom. Linkers: 3 c1cc(C2=NN=N[N]2)ccc1C1=NN=N[N]1. Metal clusters: 1 N1=N[Zn]234(N=N[Zn]1N=N2)N=N[Zn](N=N3)N=N4. The MOF has largest included sphere 7.10 A, density 0.88 g/cm3, surface area 3917.79 m2/g, accessible volume 0.73 cm3/g