CdH3(CN2)4 crystallizes in the monoclinic P2_1/c space group. Cd(1) is bonded to one N(1), one N(2), one N(3), one N(5), and two equivalent N(6) atoms to form distorted edge-sharing CdN6 pentagonal pyramids. The Cd(1)-N(1) bond length is 2.38 Å. The Cd(1)-N(2) bond length is 2.46 Å. The Cd(1)-N(3) bond length is 2.35 Å. The Cd(1)-N(5) bond length is 2.33 Å. There is one shorter (2.33 Å) and one longer (2.37 Å) Cd(1)-N(6) bond length. There are four inequivalent C sites. In the first C site, C(1) is bonded in a distorted trigonal planar geometry to one C(1), one N(1), and one N(2) atom. The C(1)-C(1) bond length is 1.49 Å. The C(1)-N(1) bond length is 1.34 Å. The C(1)-N(2) bond length is 1.34 Å. In the second C site, C(2) is bonded in a distorted trigonal planar geometry to one N(2) and one H(1) atom. The C(2)-N(2) bond length is 1.34 Å. The C(2)-H(1) bond length is 1.09 Å. In the third C site, C(3) is bonded in a distorted single-bond geometry to one C(4) and one H(2) atom. The C(3)-C(4) bond length is 1.39 Å. The C(3)-H(2) bond length is 1.09 Å. In the fourth C site, C(4) is bonded in a distorted trigonal planar geometry to one C(3), one N(1), and one H(3) atom. The C(4)-N(1) bond length is 1.34 Å. The C(4)-H(3) bond length is 1.09 Å. There are eight inequivalent N sites. In the first N site, N(1) is bonded in a trigonal planar geometry to one Cd(1), one C(1), and one C(4) atom. In the second N site, N(2) is bonded in a distorted trigonal planar geometry to one Cd(1), one C(1), and one C(2) atom. In the third N site, N(3) is bonded in a bent 120 degrees geometry to one Cd(1) and one N(4) atom. The N(3)-N(4) bond length is 1.18 Å. In the fourth N site, N(4) is bonded in a linear geometry to one N(3) and one N(5) atom. The N(4)-N(5) bond length is 1.18 Å. In the fifth N site, N(8) is bonded in a single-bond geometry to one N(7) atom. The N(8)-N(7) bond length is 1.16 Å. In the sixth N site, N(5) is bonded in a bent 150 degrees geometry to one Cd(1) and one N(4) atom. In the seventh N site, N(6) is bonded in a trigonal planar geometry to two equivalent Cd(1) and one N(7) atom. The N(6)-N(7) bond length is 1.21 Å. In the eighth N site, N(7) is bonded in a linear geometry to one N(6) and one N(8) atom. There are three inequivalent H sites. In the first H site, H(1) is bonded in a single-bond geometry to one C(2) atom. In the second H site, H(2) is bonded in a single-bond geometry to one C(3) atom. In the third H site, H(3) is bonded in a single-bond geometry to one C(4) atom. Linkers: 2 c1cnc(-c2ncccn2)nc1. Metal clusters: 4 [Cd]. The MOF has largest included sphere 1.73 A, density 2.40 g/cm3, surface area 3204.41 m2/g, accessible volume 0.07 cm3/g