TlC7NH6O2 is Indium-like structured and crystallizes in the orthorhombic Iba2 space group. The structure is zero-dimensional and consists of eight TlC7NH6O2 clusters. Tl(1) is bonded in a 1-coordinate geometry to one O(2) atom. The Tl(1)-O(2) bond length is 2.77 Å. There are seven inequivalent C sites. In the first C site, C(3) is bonded in a distorted trigonal planar geometry to one C(2), one C(4), and one H(3) atom. The C(3)-C(2) bond length is 1.41 Å. The C(3)-C(4) bond length is 1.39 Å. The C(3)-H(3) bond length is 1.09 Å. In the second C site, C(4) is bonded in a distorted trigonal planar geometry to one C(3), one C(5), and one H(4) atom. The C(4)-C(5) bond length is 1.41 Å. The C(4)-H(4) bond length is 1.09 Å. In the third C site, C(5) is bonded in a distorted trigonal planar geometry to one C(4), one C(6), and one N(1) atom. The C(5)-C(6) bond length is 1.42 Å. The C(5)-N(1) bond length is 1.38 Å. In the fourth C site, C(6) is bonded in a distorted single-bond geometry to one C(5), one C(7), and one H(5) atom. The C(6)-C(7) bond length is 1.39 Å. The C(6)-H(5) bond length is 1.09 Å. In the fifth C site, C(2) is bonded in a trigonal planar geometry to one C(1), one C(3), and one C(7) atom. The C(2)-C(1) bond length is 1.49 Å. The C(2)-C(7) bond length is 1.41 Å. In the sixth C site, C(7) is bonded in a distorted trigonal planar geometry to one C(2), one C(6), and one H(6) atom. The C(7)-H(6) bond length is 1.09 Å. In the seventh C site, C(1) is bonded in a distorted bent 120 degrees geometry to one C(2), one O(1), and one O(2) atom. The C(1)-O(1) bond length is 1.28 Å. The C(1)-O(2) bond length is 1.29 Å. N(1) is bonded in a distorted trigonal non-coplanar geometry to one C(5), one H(1), and one H(2) atom. The N(1)-H(1) bond length is 1.03 Å. The N(1)-H(2) bond length is 1.02 Å. There are six inequivalent H sites. In the first H site, H(1) is bonded in a single-bond geometry to one N(1) atom. In the second H site, H(2) is bonded in a single-bond geometry to one N(1) 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(6) is bonded in a single-bond geometry to one C(7) atom. In the fifth H site, H(4) is bonded in a single-bond geometry to one C(4) atom. In the sixth H site, H(5) is bonded in a single-bond geometry to one C(6) atom. There are two inequivalent O sites. In the first O site, O(1) is bonded in a single-bond geometry to one C(1) atom. In the second O site, O(2) is bonded in a single-bond geometry to one Tl(1) and one C(1) atom. Linkers: 4 Nc1ccc(C([O])=O)cc1. Metal clusters: 4 [Tl]. The MOF has largest included sphere 2.24 A, density 2.95 g/cm3, surface area 2509.34 m2/g, accessible volume 0.07 cm3/g