MnH4(CN)8 is Indium-like structured and crystallizes in the triclinic P-1 space group. The structure is zero-dimensional and consists of one MnH4(CN)8 cluster. There are two inequivalent Mn sites. In the first Mn site, Mn(1) is bonded in a distorted T-shaped geometry to one N(10), one N(2), and one N(7) atom. The Mn(1)-N(10) bond length is 2.25 Å. The Mn(1)-N(2) bond length is 2.27 Å. The Mn(1)-N(7) bond length is 2.26 Å. In the second Mn site, Mn(2) is bonded in an octahedral geometry to two equivalent N(11), two equivalent N(3), and two equivalent N(6) atoms. Both Mn(2)-N(11) bond lengths are 2.26 Å. Both Mn(2)-N(3) bond lengths are 2.26 Å. Both Mn(2)-N(6) bond lengths are 2.21 Å. There are twelve 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 1.48 Å. The C(1)-N(1) bond length is 1.34 Å. The C(1)-N(4) bond length is 1.33 Å. In the second C site, C(2) is bonded in a trigonal planar geometry to one C(1), one C(3), and one C(4) atom. The C(2)-C(3) bond length is 1.36 Å. The C(2)-C(4) bond length is 1.39 Å. In the third C site, C(3) is bonded in a distorted single-bond geometry to one C(2) and one H(1) atom. The C(3)-H(1) bond length is 0.93 Å. In the fourth C site, C(4) is bonded in a single-bond geometry to one C(2) and one H(2) atom. The C(4)-H(2) bond length is 0.93 Å. In the fifth C site, C(5) is bonded in a distorted trigonal planar geometry to one C(6), one N(5), and one N(8) atom. The C(5)-C(6) bond length is 1.46 Å. The C(5)-N(5) bond length is 1.34 Å. The C(5)-N(8) bond length is 1.35 Å. In the sixth C site, C(6) is bonded in a trigonal planar geometry to one C(5), one C(7), and one C(8) atom. The C(6)-C(7) bond length is 1.39 Å. The C(6)-C(8) bond length is 1.37 Å. In the seventh C site, C(7) is bonded in a distorted single-bond geometry to one C(6) and one H(3) atom. The C(7)-H(3) bond length is 0.93 Å. In the eighth C site, C(8) is bonded in a distorted single-bond geometry to one C(6) and one H(4) atom. The C(8)-H(4) bond length is 0.93 Å. In the ninth C site, C(9) is bonded in a distorted trigonal planar geometry to one C(10), one N(12), and one N(9) atom. The C(9)-C(10) bond length is 1.47 Å. The C(9)-N(12) bond length is 1.34 Å. The C(9)-N(9) bond length is 1.32 Å. In the tenth C site, C(10) is bonded in a trigonal planar geometry to one C(11), one C(12), and one C(9) atom. The C(10)-C(11) bond length is 1.39 Å. The C(10)-C(12) bond length is 1.38 Å. In the eleventh C site, C(11) is bonded in a distorted single-bond geometry to one C(10) and one H(5) atom. The C(11)-H(5) bond length is 0.93 Å. In the twelfth C site, C(12) is bonded in a distorted single-bond geometry to one C(10) and one H(6) atom. The C(12)-H(6) bond length is 0.93 Å. There are twelve inequivalent N sites. In the first N site, N(1) is bonded in a distorted water-like 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 planar geometry to one Mn(1), 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 distorted trigonal planar geometry to one Mn(2), one N(2), and one N(4) atom. The N(3)-N(4) bond length is 1.33 Å. In the fourth N site, N(4) is bonded in a water-like geometry to one C(1) and one N(3) atom. In the fifth N site, N(5) is bonded in a water-like geometry to one C(5) and one N(6) atom. The N(5)-N(6) bond length is 1.34 Å. In the sixth N site, N(6) is bonded in a distorted trigonal planar geometry to one Mn(2), one N(5), and one N(7) atom. The N(6)-N(7) bond length is 1.32 Å. In the seventh N site, N(7) is bonded in a distorted trigonal planar geometry to one Mn(1), one N(6), and one N(8) atom. The N(7)-N(8) bond length is 1.33 Å. In the eighth N site, N(8) is bonded in a distorted single-bond geometry to one C(5) and one N(7) atom. In the ninth N site, N(9) is bonded in a distorted single-bond geometry to one C(9) and one N(10) atom. The N(9)-N(10) bond length is 1.33 Å. In the tenth N site, N(10) is bonded in a distorted trigonal planar geometry to one Mn(1), one N(11), and one N(9) atom. The N(10)-N(11) bond length is 1.33 Å. In the eleventh N site, N(11) is bonded in a distorted trigonal planar geometry to one Mn(2), one N(10), and one N(12) atom. The N(11)-N(12) bond length is 1.33 Å. In the twelfth N site, N(12) is bonded in a water-like geometry to one C(9) and one N(11) atom. There are six inequivalent H sites. In the first H site, H(1) is bonded in a single-bond geometry to one C(3) atom. In the second H site, H(2) is bonded in a single-bond geometry to one C(4) atom. In the third H site, H(3) is bonded in a single-bond geometry to one C(7) atom. In the fourth H site, H(4) is bonded in a single-bond geometry to one C(8) atom. In the fifth H site, H(5) is bonded in a single-bond geometry to one C(11) atom. In the sixth H site, H(6) is bonded in a single-bond geometry to one C(12) atom. Linkers: 2 c1cc(C2=NN=N[N]2)ccc1C1=NN=N[N]1 ,1 c1cc(C2=N[N]N=N2)ccc1C1=N[N]N=N1. Metal clusters: 1 [N]1[N][Mn]234([N][N][Mn](N=N2)N=N3)N=N[Mn]1N=N4. The MOF has largest included sphere 7.14 A, density 0.82 g/cm3, surface area 4255.00 m2/g, accessible volume 0.91 cm3/g