Cu3C10N2H8SI3 crystallizes in the triclinic P-1 space group. There are three inequivalent Cu sites. In the first Cu site, Cu(1) is bonded to one S(1), one I(2), and two equivalent I(1) atoms to form distorted edge-sharing CuSI3 tetrahedra. The Cu(1)-S(1) bond length is 2.37 Å. The Cu(1)-I(2) bond length is 2.58 Å. There is one shorter (2.66 Å) and one longer (2.68 Å) Cu(1)-I(1) bond length. In the second Cu site, Cu(2) is bonded in a 4-coordinate geometry to one N(2), one S(1), and two equivalent I(2) atoms. The Cu(2)-N(2) bond length is 2.03 Å. The Cu(2)-S(1) bond length is 2.27 Å. There is one shorter (2.68 Å) and one longer (2.75 Å) Cu(2)-I(2) bond length. In the third Cu site, Cu(3) is bonded in a 4-coordinate geometry to one S(1), one I(1), and two equivalent I(3) atoms. The Cu(3)-S(1) bond length is 2.29 Å. The Cu(3)-I(1) bond length is 2.75 Å. Both Cu(3)-I(3) bond lengths are 2.61 Å. There are ten 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 H(1) atom. The C(1)-C(2) bond length is 1.37 Å. The C(1)-N(1) bond length is 1.37 Å. The C(1)-H(1) bond length is 1.09 Å. In the second C site, C(2) is bonded in a distorted trigonal planar geometry to one C(1), one C(3), and one H(2) atom. The C(2)-C(3) bond length is 1.42 Å. The C(2)-H(2) bond length is 1.09 Å. In the third C site, C(3) is bonded in a trigonal planar geometry to one C(2), one C(4), and one S(1) atom. The C(3)-C(4) bond length is 1.42 Å. The C(3)-S(1) bond length is 1.74 Å. In the fourth C site, C(4) is bonded in a distorted single-bond geometry to one C(3), one C(5), and one H(3) atom. The C(4)-C(5) bond length is 1.37 Å. The C(4)-H(3) bond length is 1.09 Å. In the fifth C site, C(5) is bonded in a distorted trigonal planar geometry to one C(4), one N(1), and one H(4) atom. The C(5)-N(1) bond length is 1.37 Å. The C(5)-H(4) bond length is 1.09 Å. In the sixth C site, C(6) is bonded in a distorted trigonal planar geometry to one C(10), one C(7), and one N(1) atom. The C(6)-C(10) bond length is 1.39 Å. The C(6)-C(7) bond length is 1.39 Å. The C(6)-N(1) bond length is 1.43 Å. In the seventh C site, C(7) is bonded in a distorted single-bond geometry to one C(6), one C(8), and one H(5) atom. The C(7)-C(8) bond length is 1.39 Å. The C(7)-H(5) bond length is 1.09 Å. In the eighth C site, C(8) is bonded in a distorted trigonal planar geometry to one C(7), one N(2), and one H(6) atom. The C(8)-N(2) bond length is 1.35 Å. The C(8)-H(6) bond length is 1.09 Å. In the ninth C site, C(9) is bonded in a distorted trigonal planar geometry to one C(10), one N(2), and one H(7) atom. The C(9)-C(10) bond length is 1.39 Å. The C(9)-N(2) bond length is 1.35 Å. The C(9)-H(7) bond length is 1.09 Å. In the tenth C site, C(10) is bonded in a distorted single-bond geometry to one C(6), one C(9), and one H(8) atom. The C(10)-H(8) bond length is 1.09 Å. There are two inequivalent N sites. In the first N site, N(1) is bonded in a trigonal planar geometry to one C(1), one C(5), and one C(6) atom. In the second N site, N(2) is bonded in a trigonal planar geometry to one Cu(2), one C(8), and one C(9) atom. There are eight 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(2) is bonded in a single-bond geometry to one C(2) atom. In the third H site, H(3) is bonded in a single-bond geometry to one C(4) atom. In the fourth H site, H(4) is bonded in a single-bond geometry to one C(5) atom. In the fifth H site, H(5) is bonded in a single-bond geometry to one C(7) atom. In the sixth H site, H(6) is bonded in a single-bond geometry to one C(8) atom. In the seventh H site, H(7) is bonded in a single-bond geometry to one C(9) atom. In the eighth H site, H(8) is bonded in a single-bond geometry to one C(10) atom. S(1) is bonded in a trigonal pyramidal geometry to one Cu(1), one Cu(2), one Cu(3), and one C(3) atom. There are three inequivalent I sites. In the first I site, I(1) is bonded in a distorted T-shaped geometry to one Cu(3) and two equivalent Cu(1) atoms. In the second I site, I(2) is bonded in a 3-coordinate geometry to one Cu(1) and two equivalent Cu(2) atoms. In the third I site, I(3) is bonded in a 2-coordinate geometry to two equivalent Cu(3) atoms. Linkers: 2 [S]C1=C[CH]N(c2ccncc2)C=C1. Metal clusters: 6 [Cu]. The MOF has largest included sphere 1.91 A, density 3.37 g/cm3, surface area 2132.80 m2/g, accessible volume 0.06 cm3/g