ZnH5(CN)3(CH3)2 crystallizes in the tetragonal I4_1/a space group. The structure consists of thirty-two 02329_fluka molecules inside a ZnH5(CN)3 framework. In the ZnH5(CN)3 framework, 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 2.01 Å. The Zn(1)-N(2) bond length is 2.02 Å. The Zn(1)-N(3) bond length is 2.05 Å. There are three inequivalent C sites. In the first C site, C(2) is bonded in a 4-coordinate geometry to one C(3), one H(10), one H(11), one H(4), and one H(5) atom. The C(2)-C(3) bond length is 1.50 Å. The C(2)-H(10) bond length is 0.97 Å. The C(2)-H(11) bond length is 0.97 Å. The C(2)-H(4) bond length is 0.97 Å. The C(2)-H(5) bond length is 0.97 Å. In the second C site, C(3) is bonded in a distorted trigonal planar geometry to one C(2), one N(2), and one N(3) atom. The C(3)-N(2) bond length is 1.32 Å. The C(3)-N(3) bond length is 1.35 Å. In the third C site, C(4) is bonded in a trigonal planar geometry to one N(1), one N(3), and one H(6) atom. The C(4)-N(1) bond length is 1.31 Å. The C(4)-N(3) bond length is 1.34 Å. The C(4)-H(6) 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(4), 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 3-coordinate geometry to one Zn(1), one C(3), and one N(1) atom. In the third N site, N(3) is bonded in a distorted trigonal planar geometry to one Zn(1), one C(3), and one C(4) atom. There are five inequivalent H sites. In the first H site, H(4) is bonded in a distorted single-bond geometry to one C(2) atom. In the second H site, H(5) is bonded in a 1-coordinate geometry to one C(2) atom. In the third H site, H(6) is bonded in a single-bond geometry to one C(4) atom. In the fourth H site, H(10) is bonded in a 1-coordinate geometry to one C(2) atom. In the fifth H site, H(11) is bonded in a distorted single-bond geometry to one C(2) atom. Linkers: 14 C.[CH3].[CH3].[C]1=NN=C[N]1 ,2 C.[CH3].[CH3].[C]1=N[N]C=N1. Metal clusters: 8 N1=N[Zn]=NN=[Zn]1. The MOF has largest included sphere 5.01 A, density 1.31 g/cm3, surface area 4214.79 m2/g, accessible volume 0.34 cm3/g