ZnH4(CN2)4CH3CHO crystallizes in the trigonal R-3 space group. The structure consists of eighteen dimethyl ether molecules inside a ZnH4(CN2)4 framework. In the ZnH4(CN2)4 framework, Zn(1) is bonded in a tetrahedral geometry to one N(1), one N(4), one N(5), and one N(8) atom. The Zn(1)-N(1) bond length is 1.99 Å. The Zn(1)-N(4) bond length is 2.04 Å. The Zn(1)-N(5) bond length is 1.99 Å. The Zn(1)-N(8) bond length is 2.03 Å. There are four inequivalent C sites. In the first C site, C(6) is bonded in a distorted trigonal planar geometry to one C(5), one N(5), and one N(8) atom. The C(6)-C(5) bond length is 1.49 Å. The C(6)-N(5) bond length is 1.34 Å. The C(6)-N(8) bond length is 1.34 Å. In the second 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 1.49 Å. The C(1)-N(1) bond length is 1.34 Å. The C(1)-N(4) bond length is 1.34 Å. In the third C site, C(2) is bonded in a distorted water-like geometry to one C(1), one H(1), and one H(2) atom. The C(2)-H(1) bond length is 1.10 Å. The C(2)-H(2) bond length is 1.10 Å. In the fourth C site, C(5) is bonded in a distorted water-like geometry to one C(6), one H(7), and one H(8) atom. The C(5)-H(7) bond length is 1.10 Å. The C(5)-H(8) bond length is 1.10 Å. There are eight inequivalent N sites. In the first N site, N(4) is bonded in a distorted trigonal planar geometry to one Zn(1), one C(1), and one N(3) atom. The N(4)-N(3) bond length is 1.36 Å. In the second N site, N(8) is bonded in a 3-coordinate geometry to one Zn(1), one C(6), and one N(7) atom. The N(8)-N(7) bond length is 1.36 Å. In the third N site, N(5) is bonded in a 3-coordinate geometry to one Zn(1), one C(6), and one N(6) atom. The N(5)-N(6) bond length is 1.36 Å. In the fourth N site, N(3) is bonded in a water-like geometry to one N(2) and one N(4) atom. The N(3)-N(2) bond length is 1.30 Å. In the fifth N site, N(6) is bonded in a water-like geometry to one N(5) and one N(7) atom. The N(6)-N(7) bond length is 1.30 Å. In the sixth N site, N(1) is bonded in a 3-coordinate geometry to one Zn(1), one C(1), and one N(2) atom. The N(1)-N(2) bond length is 1.37 Å. In the seventh N site, N(7) is bonded in a water-like geometry to one N(6) and one N(8) atom. In the eighth N site, N(2) is bonded in a water-like geometry to one N(1) and one N(3) atom. There are four 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(7) is bonded in a single-bond geometry to one C(5) atom. In the third H site, H(2) is bonded in a single-bond geometry to one C(2) atom. In the fourth H site, H(8) is bonded in a single-bond geometry to one C(5) atom. Linkers: 6 C(CC1=NN=N[N]1)OCCC1=NN=N[N]1. Metal clusters: 6 [Zn]. The MOF has largest included sphere 7.46 A, density 1.15 g/cm3, surface area 4235.70 m2/g, accessible volume 0.46 cm3/g