ZnC2H8(NBr)2 is Indium-like structured and crystallizes in the orthorhombic Ima2 space group. The structure is zero-dimensional and consists of eight ZnC2H8(NBr)2 clusters. In four of the ZnC2H8(NBr)2 clusters, Zn(1) is bonded in a tetrahedral geometry to two equivalent N(1), one Br(1), and one Br(2) atom. Both Zn(1)-N(1) bond lengths are 2.07 Å. The Zn(1)-Br(1) bond length is 2.40 Å. The Zn(1)-Br(2) bond length is 2.43 Å. C(1) is bonded in a distorted trigonal non-coplanar geometry to one N(1), one H(5), and one H(6) atom. The C(1)-N(1) bond length is 1.48 Å. The C(1)-H(5) bond length is 1.10 Å. The C(1)-H(6) bond length is 1.10 Å. N(1) is bonded to one Zn(1), one C(1), one H(1), and one H(2) atom to form distorted corner-sharing NZnH2C tetrahedra. The N(1)-H(1) bond length is 1.03 Å. The N(1)-H(2) bond length is 1.03 Å. There are four 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(5) is bonded in a single-bond geometry to one C(1) atom. In the fourth H site, H(6) is bonded in a single-bond geometry to one C(1) atom. There are two inequivalent Br sites. In the first Br site, Br(1) is bonded in a single-bond geometry to one Zn(1) atom. In the second Br site, Br(2) is bonded in a single-bond geometry to one Zn(1) atom. In four of the ZnC2H8(NBr)2 clusters, Zn(2) is bonded in a tetrahedral geometry to two equivalent N(2) and two equivalent Br(3) atoms. Both Zn(2)-N(2) bond lengths are 2.07 Å. Both Zn(2)-Br(3) bond lengths are 2.41 Å. C(2) is bonded in a distorted trigonal non-coplanar geometry to one N(2) and two equivalent H(7,8) atoms. The C(2)-N(2) bond length is 1.48 Å. Both C(2)-H(7,8) bond lengths are 1.10 Å. N(2) is bonded to one Zn(2), one C(2), one H(3), and one H(4) atom to form distorted corner-sharing NZnH2C tetrahedra. The N(2)-H(3) bond length is 1.03 Å. The N(2)-H(4) bond length is 1.03 Å. There are three inequivalent H sites. In the first H site, H(7,8) is bonded in a single-bond geometry to one C(2) atom. In the second H site, H(3) is bonded in a single-bond geometry to one N(2) atom. In the third H site, H(4) is bonded in a single-bond geometry to one N(2) atom. Br(3) is bonded in a single-bond geometry to one Zn(2) atom. Linkers: 4 NCCN. Metal clusters: 4 [Zn]. The MOF has largest included sphere 1.42 A, density 2.79 g/cm3, surface area 3110.78 m2/g, accessible volume 0.08 cm3/g