Cu2C4N3H6I crystallizes in the tetragonal I4_1/a space group. There are two inequivalent Cu sites. In the first Cu site, Cu(1) is bonded in a distorted single-bond geometry to one N(1) and three equivalent I(1) atoms. The Cu(1)-N(1) bond length is 1.99 Å. There are a spread of Cu(1)-I(1) bond distances ranging from 2.59-2.83 Å. In the second Cu site, Cu(2) is bonded in a distorted bent 150 degrees geometry to one N(2), one N(3), and two equivalent I(1) atoms. The Cu(2)-N(2) bond length is 1.88 Å. The Cu(2)-N(3) bond length is 1.88 Å. There is one shorter (3.26 Å) and one longer (3.29 Å) Cu(2)-I(1) bond length. There are four inequivalent C sites. In the first C site, C(1) is bonded in a trigonal planar geometry to one C(4), one N(1), and one N(2) atom. The C(1)-C(4) bond length is 1.49 Å. The C(1)-N(1) 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(3), one N(2), and one N(3) atom. The C(2)-C(3) bond length is 1.51 Å. The C(2)-N(2) bond length is 1.34 Å. The C(2)-N(3) bond length is 1.33 Å. In the third C site, C(3) is bonded in a trigonal non-coplanar geometry to one C(2) and three equivalent H(1,2,3) atoms. All C(3)-H(1,2,3) bond lengths are 0.98 Å. In the fourth C site, C(4) is bonded in a trigonal non-coplanar geometry to one C(1) and three equivalent H(4,5,6) atoms. All C(4)-H(4,5,6) bond lengths are 0.98 Å. There are three inequivalent N sites. In the first N site, N(1) is bonded in a 3-coordinate geometry to one Cu(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 trigonal planar geometry to one Cu(2), one C(1), and one C(2) atom. In the third N site, N(3) is bonded in a distorted trigonal planar geometry to one Cu(2), one C(2), and one N(1) atom. There are two inequivalent H sites. In the first H site, H(1,2,3) is bonded in a single-bond geometry to one C(3) atom. In the second H site, H(4,5,6) is bonded in a single-bond geometry to one C(4) atom. I(1) is bonded in a 5-coordinate geometry to two equivalent Cu(2) and three equivalent Cu(1) atoms. Linkers: 3 CC1=NN=C(C)[N]1 ,4 CC1=NC(C)=N[N]1 ,1 CC1=[N]=C(N=N1)C. Metal clusters: 2 [Cu]/N=N\[Cu]12(I)[Cu]3(I)(/N=N\[Cu])[Cu]1(I)(/N=N\[Cu])[Cu]23(I)/N=N\[Cu]. The MOF has largest included sphere 8.65 A, density 1.65 g/cm3, surface area 2599.63 m2/g, accessible volume 0.38 cm3/g