In5C3H3(NS4)2 crystallizes in the orthorhombic Pbca space group. The structure consists of a In5C3H3(NS4)2 framework. There are ten inequivalent In sites. In the first In site, In(1) is bonded to one N(3), one S(1), one S(2), and one S(3) atom to form corner-sharing InS3N tetrahedra. The In(1)-N(3) bond length is 2.18 Å. The In(1)-S(1) bond length is 2.41 Å. The In(1)-S(2) bond length is 2.42 Å. The In(1)-S(3) bond length is 2.43 Å. In the second In site, In(2) is bonded to one S(1), one S(4), one S(5), and one S(7) atom to form InS4 tetrahedra that share  a cornercorner with one In(1)S3N tetrahedra,  a cornercorner with one In(5)S3N tetrahedra,  a cornercorner with one In(3)S4 tetrahedra,  a cornercorner with one In(4)S4 tetrahedra,  a cornercorner with one In(6)S4 tetrahedra, and  a cornercorner with one In(8)S4 tetrahedra. The In(2)-S(1) bond length is 2.41 Å. The In(2)-S(4) bond length is 2.41 Å. The In(2)-S(5) bond length is 2.51 Å. The In(2)-S(7) bond length is 2.51 Å. In the third In site, In(3) is bonded to one S(2), one S(5), one S(6), and one S(8) atom to form InS4 tetrahedra that share  a cornercorner with one In(1)S3N tetrahedra,  a cornercorner with one In(7)S3N tetrahedra,  a cornercorner with one In(2)S4 tetrahedra,  a cornercorner with one In(4)S4 tetrahedra,  a cornercorner with one In(6)S4 tetrahedra, and  a cornercorner with one In(9)S4 tetrahedra. The In(3)-S(2) bond length is 2.40 Å. The In(3)-S(5) bond length is 2.50 Å. The In(3)-S(6) bond length is 2.41 Å. The In(3)-S(8) bond length is 2.50 Å. In the fourth In site, In(4) is bonded to one S(3), one S(7), one S(8), and one S(9) atom to form InS4 tetrahedra that share  a cornercorner with one In(1)S3N tetrahedra,  a cornercorner with one In(10)S3N tetrahedra,  a cornercorner with one In(2)S4 tetrahedra,  a cornercorner with one In(3)S4 tetrahedra,  a cornercorner with one In(8)S4 tetrahedra, and  a cornercorner with one In(9)S4 tetrahedra. The In(4)-S(3) bond length is 2.41 Å. The In(4)-S(7) bond length is 2.52 Å. The In(4)-S(8) bond length is 2.51 Å. The In(4)-S(9) bond length is 2.40 Å. In the fifth In site, In(5) is bonded to one N(2), one S(10), one S(12), and one S(4) atom to form corner-sharing InS3N tetrahedra. The In(5)-N(2) bond length is 2.16 Å. The In(5)-S(10) bond length is 2.42 Å. The In(5)-S(12) bond length is 2.41 Å. The In(5)-S(4) bond length is 2.43 Å. In the sixth In site, In(6) is bonded to one S(10), one S(11), one S(13), and one S(5) atom to form InS4 tetrahedra that share  a cornercorner with one In(5)S3N tetrahedra,  a cornercorner with one In(7)S3N tetrahedra,  a cornercorner with one In(2)S4 tetrahedra,  a cornercorner with one In(3)S4 tetrahedra,  a cornercorner with one In(8)S4 tetrahedra, and  a cornercorner with one In(9)S4 tetrahedra. The In(6)-S(10) bond length is 2.40 Å. The In(6)-S(11) bond length is 2.41 Å. The In(6)-S(13) bond length is 2.51 Å. The In(6)-S(5) bond length is 2.51 Å. In the seventh In site, In(7) is bonded to one N(1), one S(11), one S(14), and one S(6) atom to form corner-sharing InS3N tetrahedra. The In(7)-N(1) bond length is 2.18 Å. The In(7)-S(11) bond length is 2.41 Å. The In(7)-S(14) bond length is 2.42 Å. The In(7)-S(6) bond length is 2.43 Å. In the eighth In site, In(8) is bonded to one S(12), one S(13), one S(15), and one S(7) atom to form InS4 tetrahedra that share  a cornercorner with one In(10)S3N tetrahedra,  a cornercorner with one In(5)S3N tetrahedra,  a cornercorner with one In(2)S4 tetrahedra,  a cornercorner with one In(4)S4 tetrahedra,  a cornercorner with one In(6)S4 tetrahedra, and  a cornercorner with one In(9)S4 tetrahedra. The In(8)-S(12) bond length is 2.40 Å. The In(8)-S(13) bond length is 2.51 Å. The In(8)-S(15) bond length is 2.42 Å. The In(8)-S(7) bond length is 2.50 Å. In the ninth In site, In(9) is bonded to one S(13), one S(14), one S(16), and one S(8) atom to form InS4 tetrahedra that share  a cornercorner with one In(10)S3N tetrahedra,  a cornercorner with one In(7)S3N tetrahedra,  a cornercorner with one In(3)S4 tetrahedra,  a cornercorner with one In(4)S4 tetrahedra,  a cornercorner with one In(6)S4 tetrahedra, and  a cornercorner with one In(8)S4 tetrahedra. The In(9)-S(13) bond length is 2.50 Å. The In(9)-S(14) bond length is 2.41 Å. The In(9)-S(16) bond length is 2.41 Å. The In(9)-S(8) bond length is 2.50 Å. In the tenth In site, In(10) is bonded to one N(4), one S(15), one S(16), and one S(9) atom to form corner-sharing InS3N tetrahedra. The In(10)-N(4) bond length is 2.19 Å. The In(10)-S(15) bond length is 2.43 Å. The In(10)-S(16) bond length is 2.42 Å. The In(10)-S(9) bond length is 2.42 Å. There are six inequivalent C sites. In the first C site, C(1) is bonded in a distorted bent 120 degrees geometry to one N(2) and one H(1) atom. The C(1)-N(2) bond length is 1.37 Å. The C(1)-H(1) bond length is 0.95 Å. In the second C site, C(2) is bonded in a distorted bent 120 degrees geometry to one N(3) and one H(2) atom. The C(2)-N(3) bond length is 1.33 Å. The C(2)-H(2) bond length is 0.95 Å. In the third C site, C(4) is bonded in a trigonal planar geometry to one N(1), one N(2), and one H(4) atom. The C(4)-N(1) bond length is 1.33 Å. The C(4)-N(2) bond length is 1.29 Å. The C(4)-H(4) bond length is 0.95 Å. In the fourth C site, C(5) is bonded in a distorted bent 120 degrees geometry to one N(4) and one H(5) atom. The C(5)-N(4) bond length is 1.36 Å. The C(5)-H(5) bond length is 0.95 Å. In the fifth C site, C(6) is bonded in a trigonal planar geometry to one N(3), one N(4), and one H(6) atom. The C(6)-N(3) bond length is 1.32 Å. The C(6)-N(4) bond length is 1.31 Å. The C(6)-H(6) bond length is 0.95 Å. In the sixth C site, C(3) is bonded in a distorted bent 120 degrees geometry to one N(1) and one H(3) atom. The C(3)-N(1) bond length is 1.36 Å. The C(3)-H(3) bond length is 0.95 Å. There are four inequivalent N sites. In the first N site, N(4) is bonded in a distorted trigonal planar geometry to one In(10), one C(5), and one C(6) atom. In the second N site, N(3) is bonded in a trigonal planar geometry to one In(1), one C(2), and one C(6) atom. In the third N site, N(1) is bonded in a trigonal planar geometry to one In(7), one C(3), and one C(4) atom. In the fourth N site, N(2) is bonded in a distorted trigonal planar geometry to one In(5), one C(1), and one C(4) 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(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(3) atom. In the fourth H site, H(4) is bonded in a single-bond geometry to one C(4) atom. In the fifth H site, H(5) is bonded in a single-bond geometry to one C(5) atom. In the sixth H site, H(6) is bonded in a single-bond geometry to one C(6) atom. There are sixteen inequivalent S sites. In the first S site, S(1) is bonded in a water-like geometry to one In(1) and one In(2) atom. In the second S site, S(2) is bonded in a water-like geometry to one In(1) and one In(3) atom. In the third S site, S(3) is bonded in a water-like geometry to one In(1) and one In(4) atom. In the fourth S site, S(4) is bonded in a water-like geometry to one In(2) and one In(5) atom. In the fifth S site, S(5) is bonded in a trigonal non-coplanar geometry to one In(2), one In(3), and one In(6) atom. In the sixth S site, S(6) is bonded in a water-like geometry to one In(3) and one In(7) atom. In the seventh S site, S(7) is bonded in a trigonal non-coplanar geometry to one In(2), one In(4), and one In(8) atom. In the eighth S site, S(8) is bonded in a trigonal non-coplanar geometry to one In(3), one In(4), and one In(9) atom. In the ninth S site, S(9) is bonded in a water-like geometry to one In(10) and one In(4) atom. In the tenth S site, S(10) is bonded in a water-like geometry to one In(5) and one In(6) atom. In the eleventh S site, S(11) is bonded in a water-like geometry to one In(6) and one In(7) atom. In the twelfth S site, S(12) is bonded in a water-like geometry to one In(5) and one In(8) atom. In the thirteenth S site, S(13) is bonded in a trigonal non-coplanar geometry to one In(6), one In(8), and one In(9) atom. In the fourteenth S site, S(14) is bonded in a water-like geometry to one In(7) and one In(9) atom. In the fifteenth S site, S(15) is bonded in a water-like geometry to one In(10) and one In(8) atom. In the sixteenth S site, S(16) is bonded in a water-like geometry to one In(10) and one In(9) atom. Linkers: 16 C1=CN=C[N]1. Metal clusters: 8 [S][In]1S[In]2S[In]([S])S[In]3S[In]4S[In](S1)S[In](S4)S[In]1S[In](S2)S[In](S3)S1. The MOF has largest included sphere 7.57 A, density 1.40 g/cm3, surface area 2233.59 m2/g, accessible volume 0.48 cm3/g