Cu2C4N3H6O2I 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 2.00 Å. There are a spread of Cu(1)-I(1) bond distances ranging from 2.60-2.94 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 (3.16 Å) and one longer (3.25 Å) Cu(2)-I(1) bond length. There are four inequivalent C sites. In the first C site, C(1) is bonded in a distorted trigonal non-coplanar geometry to one C(3), one H(1), one H(2), and one O(1) atom. The C(1)-C(3) bond length is 1.48 Å. The C(1)-H(1) bond length is 1.10 Å. The C(1)-H(2) bond length is 1.10 Å. The C(1)-O(1) bond length is 1.44 Å. In the second C site, C(2) is bonded in a distorted trigonal non-coplanar geometry to one C(4), one H(3), one H(4), and one O(2) atom. The C(2)-C(4) bond length is 1.49 Å. The C(2)-H(3) bond length is 1.11 Å. The C(2)-H(4) bond length is 1.10 Å. The C(2)-O(2) bond length is 1.44 Å. In the third C site, C(3) is bonded in a distorted trigonal planar geometry to one C(1), one N(1), and one N(3) atom. The C(3)-N(1) bond length is 1.34 Å. The C(3)-N(3) bond length is 1.36 Å. In the fourth C site, C(4) is bonded in a distorted trigonal planar geometry to one C(2), one N(2), and one N(3) atom. The C(4)-N(2) bond length is 1.34 Å. The C(4)-N(3) bond length is 1.36 Å. There are three inequivalent N sites. In the first N site, N(3) is bonded in a trigonal planar geometry to one Cu(2), one C(3), and one C(4) atom. In the second N site, N(1) is bonded in a 3-coordinate geometry to one Cu(1), one C(3), and one N(2) atom. The N(1)-N(2) bond length is 1.37 Å. In the third N site, N(2) is bonded in a distorted trigonal planar geometry to one Cu(2), one C(4), and one N(1) atom. There are six 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(5) is bonded in a single-bond geometry to one O(1) atom. The H(5)-O(1) bond length is 0.97 Å. In the third H site, H(2) is bonded in a single-bond geometry to one C(1) atom. In the fourth H site, H(6) is bonded in a single-bond geometry to one O(2) atom. The H(6)-O(2) bond length is 0.97 Å. In the fifth H site, H(3) is bonded in a single-bond geometry to one C(2) atom. In the sixth H site, H(4) is bonded in a single-bond geometry to one C(2) atom. There are two inequivalent O sites. In the first O site, O(1) is bonded in a water-like geometry to one C(1) and one H(5) atom. In the second O site, O(2) is bonded in a water-like geometry to one C(2) and one H(6) atom. I(1) is bonded in a 5-coordinate geometry to two equivalent Cu(2) and three equivalent Cu(1) atoms. Linkers: 2 OCC1=[N]=C(N=N1)CO ,4 OCC1=NC(CO)=N[N]1 ,2 OCC1=NN=C(CO)[N]1. 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 6.28 A, density 1.85 g/cm3, surface area 2670.27 m2/g, accessible volume 0.24 cm3/g