Zn7H36(CN2)24 crystallizes in the cubic I-43d space group. There are two inequivalent Zn sites. In the first Zn site, Zn(1) is bonded in a tetrahedral geometry to four equivalent N(1) atoms. All Zn(1)-N(1) bond lengths are 1.97 Å. In the second Zn site, Zn(2) is bonded in a trigonal planar geometry to three equivalent N(2) atoms. All Zn(2)-N(2) bond lengths are 2.00 Å. There are two 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(2) atom. The C(1)-C(2) bond length is 1.47 Å. The C(1)-N(1) bond length is 1.33 Å. The C(1)-N(2) bond length is 1.35 Å. In the second C site, C(2) is bonded in a trigonal non-coplanar geometry to one C(1) and three equivalent H(1,2,3) atoms. All C(2)-H(1,2,3) bond lengths are 0.96 Å. There are four inequivalent N sites. In the first 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 second N site, N(2) is bonded in a distorted trigonal planar geometry to one Zn(2), one C(1), and one N(4) atom. The N(2)-N(4) bond length is 1.30 Å. In the third N site, N(3) is bonded in a distorted water-like geometry to one N(1) and one N(4) atom. The N(3)-N(4) bond length is 1.29 Å. In the fourth N site, N(4) is bonded in a water-like geometry to one N(2) and one N(3) atom. H(1,2,3) is bonded in a single-bond geometry to one C(2) atom. Linkers: 46 CC1=NN=N[N]1 ,2 CC1=N[N]N=N1. Metal clusters: 28 [Zn]. The MOF has largest included sphere 6.78 A, density 0.86 g/cm3, surface area 4371.70 m2/g, accessible volume 0.80 cm3/g