Zn2H6(CN6)3 crystallizes in the trigonal R-3c space group. The structure consists of a Zn2H6(CN6)3 framework. Zn(1) is bonded in a tetrahedral geometry to one N(5) and three equivalent N(1) atoms. The Zn(1)-N(5) bond length is 1.99 Å. All Zn(1)-N(1) bond lengths are 1.98 Å. C(1) is bonded in a trigonal planar geometry to one N(2) and two equivalent N(1) atoms. The C(1)-N(2) bond length is 1.33 Å. Both C(1)-N(1) bond lengths are 1.36 Å. There are five inequivalent N sites. In the first N site, N(4) is bonded in a linear geometry to two equivalent N(5) atoms. Both N(4)-N(5) bond lengths are 1.17 Å. In the second N site, N(1) is bonded in a distorted trigonal planar geometry to one Zn(1), one C(1), and one N(3) atom. The N(1)-N(3) bond length is 1.37 Å. In the third N site, N(5) is bonded in a linear geometry to one Zn(1) and one N(4) atom. In the fourth N site, N(2) is bonded in a trigonal planar geometry to one C(1) and two equivalent H(1) atoms. Both N(2)-H(1) bond lengths are 1.03 Å. In the fifth N site, N(3) is bonded in a water-like geometry to one N(1) and one N(3) atom. The N(3)-N(3) bond length is 1.29 Å. H(1) is bonded in a single-bond geometry to one N(2) atom. Linkers: 6 NC1=NN=N[N]1. Metal clusters: 4 [Zn]. The MOF has largest included sphere 1.71 A, density 2.13 g/cm3, surface area 3512.68 m2/g, accessible volume 0.12 cm3/g