Cu2CN4HI crystallizes in the orthorhombic Pbam space group. There are two inequivalent Cu sites. In the first Cu site, Cu(1) is bonded in a distorted bent 120 degrees geometry to two equivalent N(1) and two equivalent I(1) atoms. Both Cu(1)-N(1) bond lengths are 1.99 Å. Both Cu(1)-I(1) bond lengths are 2.64 Å. In the second Cu site, Cu(2) is bonded in a distorted bent 150 degrees geometry to two equivalent N(2) and two equivalent I(1) atoms. Both Cu(2)-N(2) bond lengths are 1.94 Å. There is one shorter (2.73 Å) and one longer (2.97 Å) Cu(2)-I(1) bond length. C(1) is bonded in a trigonal planar geometry to two equivalent N(2) and one H(1) atom. Both C(1)-N(2) bond lengths are 1.34 Å. The C(1)-H(1) bond length is 1.08 Å. There are two inequivalent N sites. In the first N site, N(1) is bonded in a distorted trigonal planar geometry to one Cu(1), one N(1), and one N(2) atom. The N(1)-N(1) bond length is 1.32 Å. The N(1)-N(2) bond length is 1.35 Å. In the second N site, N(2) is bonded in a 3-coordinate geometry to one Cu(2), one C(1), and one N(1) atom. H(1) is bonded in a single-bond geometry to one C(1) atom. I(1) is bonded to two equivalent Cu(1) and two equivalent Cu(2) atoms to form a mixture of distorted edge and corner-sharing ICu4 tetrahedra. Linkers: 4 C1=NN=N[N]1. Metal clusters: 8 [Cu]. The MOF has largest included sphere 1.95 A, density 4.05 g/cm3, surface area 1901.60 m2/g, accessible volume 0.05 cm3/g