MoNi2H24(CN)16(CH2)16 crystallizes in the orthorhombic Fddd space group. The structure consists of one hundred and twenty-eight 02329_fluka molecules inside a MoNi2H24(CN)16 framework. In the MoNi2H24(CN)16 framework, Mo(1) is bonded in a 8-coordinate geometry to four equivalent C(1) and four equivalent C(2) atoms. All Mo(1)-C(1) bond lengths are 2.10 Å. All Mo(1)-C(2) bond lengths are 2.16 Å. Ni(1) is bonded in an octahedral geometry to two equivalent N(1), two equivalent N(3), and two equivalent N(4) atoms. Both Ni(1)-N(1) bond lengths are 1.96 Å. Both Ni(1)-N(3) bond lengths are 2.14 Å. Both Ni(1)-N(4) bond lengths are 2.13 Å. There are four inequivalent C sites. In the first C site, C(2) is bonded in a distorted linear geometry to one Mo(1) and one N(2) atom. The C(2)-N(2) bond length is 1.18 Å. In the second C site, C(1) is bonded in a linear geometry to one Mo(1) and one N(1) atom. The C(1)-N(1) bond length is 1.17 Å. In the third C site, C(3) is bonded in a distorted water-like geometry to one N(3) and one H(1) atom. The C(3)-N(3) bond length is 1.48 Å. The C(3)-H(1) bond length is 1.10 Å. In the fourth C site, C(8) is bonded in a distorted water-like geometry to one N(4) and one H(10) atom. The C(8)-N(4) bond length is 1.48 Å. The C(8)-H(10) bond length is 1.10 Å. There are four inequivalent N sites. In the first N site, N(2) is bonded in a single-bond geometry to one C(2) atom. In the second N site, N(3) is bonded to one Ni(1), one C(3), one H(11), and one H(12) atom to form distorted corner-sharing NNiH2C tetrahedra. The N(3)-H(11) bond length is 1.03 Å. The N(3)-H(12) bond length is 1.02 Å. In the third N site, N(1) is bonded in a bent 150 degrees geometry to one Ni(1) and one C(1) atom. In the fourth N site, N(4) is bonded to one Ni(1), one C(8), one H(13), and one H(14) atom to form distorted corner-sharing NNiH2C tetrahedra. The N(4)-H(13) bond length is 1.02 Å. The N(4)-H(14) bond length is 1.02 Å. There are six inequivalent H sites. In the first H site, H(10) is bonded in a single-bond geometry to one C(8) atom. In the second H site, H(14) is bonded in a single-bond geometry to one N(4) atom. In the third H site, H(11) is bonded in a single-bond geometry to one N(3) atom. In the fourth H site, H(12) is bonded in a single-bond geometry to one N(3) atom. In the fifth H site, H(1) is bonded in a single-bond geometry to one C(3) atom. In the sixth H site, H(13) is bonded in a single-bond geometry to one N(4) atom. Linkers: 3 N[C@H]1CCCC[C@@H]1N ,3 N[C@@H]1CCCC[C@H]1N. Metal clusters: 4 [Ni] ,2 [Mo]. The MOF has largest included sphere 4.34 A, density 0.99 g/cm3, surface area 5174.14 m2/g, accessible volume 0.54 cm3/g