CsC4N11H4O crystallizes in the triclinic P-1 space group. There are two inequivalent Cs sites. In the first Cs site, Cs(1) is bonded in a 11-coordinate geometry to one N(13), one N(17), one N(19), one N(7), one N(8), one N(9), two equivalent N(18), one H(1), one O(1), and one O(2) atom. The Cs(1)-N(13) bond length is 3.43 Å. The Cs(1)-N(17) bond length is 3.22 Å. The Cs(1)-N(19) bond length is 3.26 Å. The Cs(1)-N(7) bond length is 3.45 Å. The Cs(1)-N(8) bond length is 3.54 Å. The Cs(1)-N(9) bond length is 3.25 Å. Both Cs(1)-N(18) bond lengths are 3.41 Å. The Cs(1)-H(1) bond length is 3.16 Å. The Cs(1)-O(1) bond length is 3.36 Å. The Cs(1)-O(2) bond length is 3.10 Å. In the second Cs site, Cs(2) is bonded in a 8-coordinate geometry to one N(13), one N(2), one N(20), one N(7), one N(8), one N(9), and two equivalent O(1) atoms. The Cs(2)-N(13) bond length is 3.40 Å. The Cs(2)-N(2) bond length is 3.25 Å. The Cs(2)-N(20) bond length is 3.19 Å. The Cs(2)-N(7) bond length is 3.47 Å. The Cs(2)-N(8) bond length is 3.37 Å. The Cs(2)-N(9) bond length is 3.25 Å. There is one shorter (3.19 Å) and one longer (3.28 Å) Cs(2)-O(1) bond length. There are eight 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 N(4) atom. The C(1)-C(2) bond length is 1.44 Å. The C(1)-N(1) bond length is 1.35 Å. The C(1)-N(4) bond length is 1.35 Å. In the second C site, C(2) is bonded in a distorted single-bond geometry to one C(1), one C(3), and one N(5) atom. The C(2)-C(3) bond length is 1.40 Å. The C(2)-N(5) bond length is 1.35 Å. In the third C site, C(3) is bonded in a distorted single-bond geometry to one C(2), one C(4), and one N(7) atom. The C(3)-C(4) bond length is 1.44 Å. The C(3)-N(7) bond length is 1.37 Å. In the fourth C site, C(4) is bonded in a distorted water-like geometry to one C(3), one N(11), and one N(8) atom. The C(4)-N(11) bond length is 1.35 Å. The C(4)-N(8) bond length is 1.34 Å. In the fifth C site, C(5) is bonded in a distorted trigonal planar geometry to one C(6), one N(12), and one N(15) atom. The C(5)-C(6) bond length is 1.44 Å. The C(5)-N(12) bond length is 1.35 Å. The C(5)-N(15) bond length is 1.35 Å. In the sixth C site, C(6) is bonded in a distorted single-bond geometry to one C(5), one C(7), and one N(16) atom. The C(6)-C(7) bond length is 1.40 Å. The C(6)-N(16) bond length is 1.36 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 N(18) atom. The C(7)-C(8) bond length is 1.44 Å. The C(7)-N(18) bond length is 1.37 Å. In the eighth C site, C(8) is bonded in a distorted water-like geometry to one C(7), one N(19), and one N(22) atom. The C(8)-N(19) bond length is 1.34 Å. The C(8)-N(22) bond length is 1.35 Å. There are twenty-two inequivalent N sites. In the first N site, N(1) is bonded in a distorted single-bond geometry to one C(1) and one N(2) atom. The N(1)-N(2) bond length is 1.34 Å. In the second N site, N(2) is bonded in a distorted trigonal non-coplanar geometry to one Cs(2), one N(1), and one N(3) atom. The N(2)-N(3) bond length is 1.32 Å. In the third N site, N(3) is bonded in a water-like geometry to one N(2) and one N(4) atom. The N(3)-N(4) bond length is 1.34 Å. In the fourth N site, N(4) is bonded in a 3-coordinate geometry to one C(1), one N(3), and one H(7) atom. The N(4)-H(7) bond length is 1.70 Å. In the fifth N site, N(5) is bonded in a 3-coordinate geometry to one C(2), one N(6), and one H(5) atom. The N(5)-N(6) bond length is 1.34 Å. The N(5)-H(5) bond length is 1.07 Å. In the sixth N site, N(6) is bonded in a water-like geometry to one N(5) and one N(7) atom. The N(6)-N(7) bond length is 1.31 Å. In the seventh N site, N(7) is bonded in a 1-coordinate geometry to one Cs(1), one Cs(2), one C(3), and one N(6) atom. In the eighth N site, N(8) is bonded in a distorted single-bond geometry to one Cs(1), one Cs(2), one C(4), and one N(9) atom. The N(8)-N(9) bond length is 1.35 Å. In the ninth N site, N(9) is bonded in a distorted tetrahedral geometry to one Cs(1), one Cs(2), one N(10), and one N(8) atom. The N(9)-N(10) bond length is 1.31 Å. In the tenth N site, N(10) is bonded in a water-like geometry to one N(11) and one N(9) atom. The N(10)-N(11) bond length is 1.34 Å. In the eleventh N site, N(11) is bonded in a 2-coordinate geometry to one C(4), one N(10), and one H(6) atom. The N(11)-H(6) bond length is 1.05 Å. In the twelfth N site, N(12) is bonded in a distorted single-bond geometry to one C(5) and one N(13) atom. The N(12)-N(13) bond length is 1.34 Å. In the thirteenth N site, N(13) is bonded in a 4-coordinate geometry to one Cs(1), one Cs(2), one N(12), and one N(14) atom. The N(13)-N(14) bond length is 1.32 Å. In the fourteenth N site, N(14) is bonded in a 2-coordinate geometry to one N(13) and one N(15) atom. The N(14)-N(15) bond length is 1.34 Å. In the fifteenth N site, N(15) is bonded in a 3-coordinate geometry to one C(5), one N(14), and one H(5) atom. The N(15)-H(5) bond length is 1.69 Å. In the sixteenth N site, N(16) is bonded in a 3-coordinate geometry to one C(6), one N(17), and one H(7) atom. The N(16)-N(17) bond length is 1.34 Å. The N(16)-H(7) bond length is 1.07 Å. In the seventeenth N site, N(17) is bonded in a 3-coordinate geometry to one Cs(1), one N(16), and one N(18) atom. The N(17)-N(18) bond length is 1.31 Å. In the eighteenth N site, N(18) is bonded in a distorted single-bond geometry to two equivalent Cs(1), one C(7), and one N(17) atom. In the nineteenth N site, N(19) is bonded in a distorted single-bond geometry to one Cs(1), one C(8), and one N(20) atom. The N(19)-N(20) bond length is 1.35 Å. In the twentieth N site, N(20) is bonded in a trigonal planar geometry to one Cs(2), one N(19), and one N(21) atom. The N(20)-N(21) bond length is 1.31 Å. In the twenty-first N site, N(21) is bonded in a water-like geometry to one N(20) and one N(22) atom. The N(21)-N(22) bond length is 1.34 Å. In the twenty-second N site, N(22) is bonded in a 2-coordinate geometry to one C(8), one N(21), and one H(8) atom. The N(22)-H(8) bond length is 1.05 Å. There are eight inequivalent H sites. In the first H site, H(1) is bonded in a single-bond geometry to one Cs(1) and one O(1) atom. The H(1)-O(1) bond length is 0.99 Å. In the second H site, H(2) is bonded in a single-bond geometry to one O(1) atom. The H(2)-O(1) bond length is 0.99 Å. In the third H site, H(3) is bonded in a single-bond geometry to one O(2) atom. The H(3)-O(2) bond length is 0.99 Å. In the fourth H site, H(4) is bonded in a single-bond geometry to one O(2) atom. The H(4)-O(2) bond length is 0.98 Å. In the fifth H site, H(5) is bonded in a distorted single-bond geometry to one N(15) and one N(5) atom. In the sixth H site, H(6) is bonded in a single-bond geometry to one N(11) atom. In the seventh H site, H(7) is bonded in a distorted single-bond geometry to one N(16) and one N(4) atom. In the eighth H site, H(8) is bonded in a single-bond geometry to one N(22) atom. There are two inequivalent O sites. In the first O site, O(1) is bonded in a water-like geometry to one Cs(1), two equivalent Cs(2), one H(1), and one H(2) atom. In the second O site, O(2) is bonded in a water-like geometry to one Cs(1), one H(3), and one H(4) atom. Linkers: 4 [N]1N=NN=C1c1[nH]nnc1-c1nnn[nH]1. Metal clusters: 4 [Cs]. The MOF has largest included sphere 1.79 A, density 2.31 g/cm3, surface area 3379.16 m2/g, accessible volume 0.11 cm3/g