Cu2C21N9H28I crystallizes in the orthorhombic Pnma space group. There are two inequivalent Cu sites. In the first Cu site, Cu(1) is bonded in a distorted trigonal non-coplanar geometry to one N(5), two equivalent N(1), and one I(1) atom. The Cu(1)-N(5) bond length is 1.90 Å. Both Cu(1)-N(1) bond lengths are 2.01 Å. The Cu(1)-I(1) bond length is 2.71 Å. In the second Cu site, Cu(2) is bonded in a 3-coordinate geometry to one C(11), two equivalent N(3), and one I(1) atom. The Cu(2)-C(11) bond length is 1.84 Å. Both Cu(2)-N(3) bond lengths are 2.01 Å. The Cu(2)-I(1) bond length is 2.94 Å. There are eleven inequivalent C sites. In the first C site, C(2) is bonded in a distorted trigonal planar geometry to one C(1), one C(3), and one N(1) atom. The C(2)-C(1) bond length is 1.49 Å. The C(2)-C(3) bond length is 1.42 Å. The C(2)-N(1) bond length is 1.34 Å. In the second C site, C(3) is bonded in a trigonal planar geometry to one C(2), one C(4), and one C(8) atom. The C(3)-C(4) bond length is 1.40 Å. The C(3)-C(8) bond length is 1.46 Å. In the third C site, C(4) is bonded in a distorted trigonal planar geometry to one C(3), one C(5), and one N(2) atom. The C(4)-C(5) bond length is 1.49 Å. The C(4)-N(2) bond length is 1.36 Å. In the fourth C site, C(5) is bonded in a distorted trigonal non-coplanar geometry to one C(4), one H(6), one H(7), and one H(8) atom. The C(5)-H(6) bond length is 1.10 Å. The C(5)-H(7) bond length is 1.10 Å. The C(5)-H(8) bond length is 1.10 Å. In the fifth C site, C(6) is bonded in a distorted trigonal non-coplanar geometry to one C(7), one H(10), one H(11), and one H(9) atom. The C(6)-C(7) bond length is 1.48 Å. The C(6)-H(10) bond length is 1.10 Å. The C(6)-H(11) bond length is 1.10 Å. The C(6)-H(9) bond length is 1.10 Å. In the sixth C site, C(7) is bonded in a distorted trigonal planar geometry to one C(6), one C(8), and one N(4) atom. The C(7)-C(8) bond length is 1.40 Å. The C(7)-N(4) bond length is 1.35 Å. In the seventh C site, C(8) is bonded in a trigonal planar geometry to one C(3), one C(7), and one C(9) atom. The C(8)-C(9) bond length is 1.42 Å. In the eighth C site, C(9) is bonded in a distorted trigonal planar geometry to one C(10), one C(8), and one N(3) atom. The C(9)-C(10) bond length is 1.49 Å. The C(9)-N(3) bond length is 1.35 Å. In the ninth C site, C(10) is bonded in a distorted trigonal non-coplanar geometry to one C(9), one H(12), one H(13), and one H(14) atom. The C(10)-H(12) bond length is 1.10 Å. The C(10)-H(13) bond length is 1.10 Å. The C(10)-H(14) bond length is 1.10 Å. In the tenth C site, C(11) is bonded in a linear geometry to one Cu(2) and one N(5) atom. The C(11)-N(5) bond length is 1.18 Å. In the eleventh C site, C(1) is bonded in a distorted trigonal non-coplanar geometry to one C(2), one H(3), one H(4), and one H(5) atom. The C(1)-H(3) bond length is 1.10 Å. The C(1)-H(4) bond length is 1.10 Å. The C(1)-H(5) bond length is 1.10 Å. There are five inequivalent N sites. In the first N site, N(1) is bonded in a 3-coordinate geometry to one Cu(1), one C(2), and one N(2) atom. The N(1)-N(2) bond length is 1.35 Å. In the second N site, N(2) is bonded in a 2-coordinate geometry to one C(4), one N(1), and one H(1) atom. The N(2)-H(1) bond length is 1.02 Å. In the third N site, N(3) is bonded in a distorted trigonal planar geometry to one Cu(2), one C(9), and one N(4) atom. The N(3)-N(4) bond length is 1.35 Å. In the fourth N site, N(4) is bonded in a 2-coordinate geometry to one C(7), one N(3), and one H(2) atom. The N(4)-H(2) bond length is 1.02 Å. In the fifth N site, N(5) is bonded in a linear geometry to one Cu(1) and one C(11) atom. There are fourteen inequivalent H sites. In the first H site, H(1) is bonded in a single-bond geometry to one N(2) atom. In the second H site, H(2) is bonded in a single-bond geometry to one N(4) atom. In the third H site, H(3) is bonded in a single-bond geometry to one C(1) atom. In the fourth H site, H(4) is bonded in a single-bond geometry to one C(1) atom. In the fifth H site, H(5) is bonded in a single-bond geometry to one C(1) atom. In the sixth H site, H(6) is bonded in a single-bond geometry to one C(5) atom. In the seventh H site, H(7) is bonded in a single-bond geometry to one C(5) atom. In the eighth H site, H(8) is bonded in a single-bond geometry to one C(5) atom. In the ninth H site, H(9) is bonded in a single-bond geometry to one C(6) atom. In the tenth H site, H(10) is bonded in a single-bond geometry to one C(6) atom. In the eleventh H site, H(11) is bonded in a single-bond geometry to one C(6) atom. In the twelfth H site, H(12) is bonded in a single-bond geometry to one C(10) atom. In the thirteenth H site, H(13) is bonded in a single-bond geometry to one C(10) atom. In the fourteenth H site, H(14) is bonded in a single-bond geometry to one C(10) atom. I(1) is bonded in a water-like geometry to one Cu(1) and one Cu(2) atom. Linkers: 8 Cc1n[nH]c(C)c1-c1c(C)n[nH]c1C. Metal clusters: 8 [Cu]. The MOF has largest included sphere 4.92 A, density 1.59 g/cm3, surface area 4435.18 m2/g, accessible volume 0.24 cm3/g