ZnH4(CN)3 crystallizes in the tetragonal I4_1/a space group. Zn(1) is bonded in a trigonal non-coplanar geometry to one N(1), one N(2), and one N(3) atom. The Zn(1)-N(1) bond length is 2.00 Å. The Zn(1)-N(2) bond length is 2.01 Å. The Zn(1)-N(3) bond length is 2.03 Å. There are three inequivalent C sites. In the first C site, C(1) is bonded in a trigonal non-coplanar geometry to one C(2); one H(1); and two equivalent H(2,3) atoms. The C(1)-C(2) bond length is 1.50 Å. The C(1)-H(1) bond length is 0.96 Å. Both C(1)-H(2,3) bond lengths are 0.96 Å. In the second C site, C(2) is bonded in a distorted trigonal planar geometry to one C(1), one N(2), and one N(3) atom. The C(2)-N(2) bond length is 1.31 Å. The C(2)-N(3) bond length is 1.35 Å. In the third C site, C(3) is bonded in a trigonal planar geometry to one N(1), one N(3), and one H(4) atom. The C(3)-N(1) bond length is 1.31 Å. The C(3)-N(3) bond length is 1.34 Å. The C(3)-H(4) bond length is 0.93 Å. There are three inequivalent N sites. In the first N site, N(1) is bonded in a distorted trigonal planar geometry to one Zn(1), one C(3), and one N(2) atom. The N(1)-N(2) bond length is 1.38 Å. In the second N site, N(2) is bonded in a distorted trigonal planar geometry to one Zn(1), one C(2), and one N(1) atom. In the third N site, N(3) is bonded in a trigonal planar geometry to one Zn(1), one C(2), and one C(3) atom. There are three inequivalent H sites. In the first H site, H(1) is bonded in a single-bond geometry to one C(1) atom. In the second H site, H(2,3) is bonded in a single-bond geometry to one C(1) atom. In the third H site, H(4) is bonded in a single-bond geometry to one C(3) atom. Linkers: 6 CC1=NN=C[N]1. Metal clusters: 2 N1=N[Zn]=NN=[Zn]1 ,4 [Zn]. The MOF has largest included sphere 6.29 A, density 1.10 g/cm3, surface area 3938.22 m2/g, accessible volume 0.62 cm3/g