CsC3H2(NS)3 crystallizes in the triclinic P1 space group. There are four inequivalent Cs sites. In the first Cs site, Cs(1) is bonded in a 8-coordinate geometry to one N(1), one N(11), one S(8), one S(9), two equivalent S(1), and two equivalent S(3) atoms. The Cs(1)-N(1) bond length is 3.24 Å. The Cs(1)-N(11) bond length is 3.08 Å. The Cs(1)-S(8) bond length is 3.48 Å. The Cs(1)-S(9) bond length is 4.02 Å. There is one shorter (3.46 Å) and one longer (3.57 Å) Cs(1)-S(1) bond length. There is one shorter (3.60 Å) and one longer (3.80 Å) Cs(1)-S(3) bond length. In the second Cs site, Cs(2) is bonded in a 6-coordinate geometry to one N(12), one N(2), one S(4), one S(7), and two equivalent S(2) atoms. The Cs(2)-N(12) bond length is 3.08 Å. The Cs(2)-N(2) bond length is 3.23 Å. The Cs(2)-S(4) bond length is 3.59 Å. The Cs(2)-S(7) bond length is 3.48 Å. There is one shorter (3.46 Å) and one longer (3.57 Å) Cs(2)-S(2) bond length. In the third Cs site, Cs(3) is bonded in a 9-coordinate geometry to one N(1), one N(11), one S(11), two equivalent S(10), two equivalent S(5), and two equivalent S(7) atoms. The Cs(3)-N(1) bond length is 3.41 Å. The Cs(3)-N(11) bond length is 3.55 Å. The Cs(3)-S(11) bond length is 3.49 Å. There is one shorter (3.82 Å) and one longer (4.06 Å) Cs(3)-S(10) bond length. There is one shorter (3.66 Å) and one longer (3.74 Å) Cs(3)-S(5) bond length. There is one shorter (3.42 Å) and one longer (3.48 Å) Cs(3)-S(7) bond length. In the fourth Cs site, Cs(4) is bonded in a 9-coordinate geometry to one N(12), one N(2), one S(12), two equivalent S(6), two equivalent S(8), and two equivalent S(9) atoms. The Cs(4)-N(12) bond length is 3.55 Å. The Cs(4)-N(2) bond length is 3.41 Å. The Cs(4)-S(12) bond length is 3.49 Å. There is one shorter (3.65 Å) and one longer (3.74 Å) Cs(4)-S(6) bond length. There is one shorter (3.42 Å) and one longer (3.48 Å) Cs(4)-S(8) bond length. There is one shorter (3.83 Å) and one longer (4.06 Å) Cs(4)-S(9) bond length. There are twelve inequivalent C sites. In the first C site, C(1) is bonded in a distorted trigonal planar geometry to one N(5), one N(9), and one S(9) atom. The C(1)-N(5) bond length is 1.37 Å. The C(1)-N(9) bond length is 1.37 Å. The C(1)-S(9) bond length is 1.67 Å. In the second C site, C(2) is bonded in a distorted trigonal planar geometry to one N(10), one N(6), and one S(10) atom. The C(2)-N(10) bond length is 1.37 Å. The C(2)-N(6) bond length is 1.37 Å. The C(2)-S(10) bond length is 1.67 Å. In the third C site, C(3) is bonded in a distorted bent 120 degrees geometry to one N(11), one N(3), and one S(7) atom. The C(3)-N(11) bond length is 1.35 Å. The C(3)-N(3) bond length is 1.38 Å. The C(3)-S(7) bond length is 1.69 Å. In the fourth C site, C(4) is bonded in a distorted bent 120 degrees geometry to one N(12), one N(4), and one S(8) atom. The C(4)-N(12) bond length is 1.35 Å. The C(4)-N(4) bond length is 1.38 Å. The C(4)-S(8) bond length is 1.69 Å. In the fifth C site, C(5) is bonded in a distorted trigonal planar geometry to one N(11), one N(7), and one S(3) atom. The C(5)-N(11) bond length is 1.35 Å. The C(5)-N(7) bond length is 1.39 Å. The C(5)-S(3) bond length is 1.68 Å. In the sixth C site, C(6) is bonded in a distorted trigonal planar geometry to one N(12), one N(8), and one S(4) atom. The C(6)-N(12) bond length is 1.35 Å. The C(6)-N(8) bond length is 1.39 Å. The C(6)-S(4) bond length is 1.68 Å. In the seventh C site, C(7) is bonded in a distorted trigonal planar geometry to one N(1), one N(9), and one S(1) atom. The C(7)-N(1) bond length is 1.35 Å. The C(7)-N(9) bond length is 1.38 Å. The C(7)-S(1) bond length is 1.69 Å. In the eighth C site, C(8) is bonded in a distorted trigonal planar geometry to one N(10), one N(2), and one S(2) atom. The C(8)-N(10) bond length is 1.38 Å. The C(8)-N(2) bond length is 1.35 Å. The C(8)-S(2) bond length is 1.69 Å. In the ninth C site, C(9) is bonded in a distorted trigonal planar geometry to one N(1), one N(5), and one S(5) atom. The C(9)-N(1) bond length is 1.35 Å. The C(9)-N(5) bond length is 1.38 Å. The C(9)-S(5) bond length is 1.69 Å. In the tenth C site, C(10) is bonded in a distorted trigonal planar geometry to one N(2), one N(6), and one S(6) atom. The C(10)-N(2) bond length is 1.35 Å. The C(10)-N(6) bond length is 1.38 Å. The C(10)-S(6) bond length is 1.69 Å. In the eleventh C site, C(11) is bonded in a distorted trigonal planar geometry to one N(3), one N(7), and one S(11) atom. The C(11)-N(3) bond length is 1.36 Å. The C(11)-N(7) bond length is 1.36 Å. The C(11)-S(11) bond length is 1.67 Å. In the twelfth C site, C(12) is bonded in a distorted trigonal planar geometry to one N(4), one N(8), and one S(12) atom. The C(12)-N(4) bond length is 1.36 Å. The C(12)-N(8) bond length is 1.36 Å. The C(12)-S(12) bond length is 1.67 Å. There are twelve inequivalent N sites. In the first N site, N(1) is bonded in a distorted bent 120 degrees geometry to one Cs(1), one Cs(3), one C(7), and one C(9) atom. In the second N site, N(2) is bonded in a distorted bent 120 degrees geometry to one Cs(2), one Cs(4), one C(10), and one C(8) atom. In the third N site, N(3) is bonded in a trigonal planar geometry to one C(11), one C(3), and one H(1) atom. The N(3)-H(1) bond length is 1.04 Å. In the fourth N site, N(4) is bonded in a trigonal planar geometry to one C(12), one C(4), and one H(2) atom. The N(4)-H(2) bond length is 1.04 Å. In the fifth N site, N(5) is bonded in a trigonal planar geometry to one C(1), one C(9), and one H(3) atom. The N(5)-H(3) bond length is 1.04 Å. In the sixth N site, N(6) is bonded in a trigonal planar geometry to one C(10), one C(2), and one H(4) atom. The N(6)-H(4) bond length is 1.04 Å. In the seventh N site, N(7) is bonded in a trigonal planar geometry to one C(11), one C(5), and one H(5) atom. The N(7)-H(5) bond length is 1.04 Å. In the eighth N site, N(8) is bonded in a trigonal planar geometry to one C(12), one C(6), and one H(6) atom. The N(8)-H(6) bond length is 1.04 Å. In the ninth N site, N(9) is bonded in a trigonal planar geometry to one C(1), one C(7), and one H(7) atom. The N(9)-H(7) bond length is 1.04 Å. In the tenth N site, N(10) is bonded in a trigonal planar geometry to one C(2), one C(8), and one H(8) atom. The N(10)-H(8) bond length is 1.04 Å. In the eleventh N site, N(11) is bonded in a distorted bent 120 degrees geometry to one Cs(1), one Cs(3), one C(3), and one C(5) atom. In the twelfth N site, N(12) is bonded in a distorted bent 120 degrees geometry to one Cs(2), one Cs(4), one C(4), and one C(6) atom. There are eight inequivalent H sites. In the first H site, H(1) is bonded in a single-bond geometry to one N(3) 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 N(5) atom. In the fourth H site, H(4) is bonded in a single-bond geometry to one N(6) atom. In the fifth H site, H(5) is bonded in a single-bond geometry to one N(7) atom. In the sixth H site, H(6) is bonded in a single-bond geometry to one N(8) atom. In the seventh H site, H(7) is bonded in a single-bond geometry to one N(9) atom. In the eighth H site, H(8) is bonded in a single-bond geometry to one N(10) atom. There are twelve inequivalent S sites. In the first S site, S(1) is bonded in a 1-coordinate geometry to two equivalent Cs(1) and one C(7) atom. In the second S site, S(2) is bonded in a 1-coordinate geometry to two equivalent Cs(2) and one C(8) atom. In the third S site, S(3) is bonded in a 2-coordinate geometry to two equivalent Cs(1) and one C(5) atom. In the fourth S site, S(4) is bonded in a 2-coordinate geometry to one Cs(2) and one C(6) atom. In the fifth S site, S(5) is bonded in a 1-coordinate geometry to two equivalent Cs(3) and one C(9) atom. In the sixth S site, S(6) is bonded in a 1-coordinate geometry to two equivalent Cs(4) and one C(10) atom. In the seventh S site, S(7) is bonded in a 4-coordinate geometry to one Cs(2), two equivalent Cs(3), and one C(3) atom. In the eighth S site, S(8) is bonded in a 4-coordinate geometry to one Cs(1), two equivalent Cs(4), and one C(4) atom. In the ninth S site, S(9) is bonded in a distorted single-bond geometry to one Cs(1), two equivalent Cs(4), and one C(1) atom. In the tenth S site, S(10) is bonded in a distorted single-bond geometry to two equivalent Cs(3) and one C(2) atom. In the eleventh S site, S(11) is bonded in a distorted bent 150 degrees geometry to one Cs(3) and one C(11) atom. In the twelfth S site, S(12) is bonded in a distorted bent 150 degrees geometry to one Cs(4) and one C(12) atom. Linkers: 4 S=C1[N]C(=S)NC(=S)N1. Metal clusters: 4 [Cs]. The MOF has largest included sphere 2.19 A, density 2.40 g/cm3, surface area 3258.91 m2/g, accessible volume 0.11 cm3/g