CuH4(C2N)4(HC2N)2 crystallizes in the tetragonal P4_32_12 space group. The structure consists of eight n-methyl methanimine molecules inside a CuH4(C2N)4 framework. In the CuH4(C2N)4 framework, Cu(1) is bonded in a 4-coordinate geometry to two equivalent N(1) and two equivalent N(2) atoms. Both Cu(1)-N(1) bond lengths are 2.01 Å. Both Cu(1)-N(2) bond lengths are 2.17 Å. There are four 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 H(1) atom. The C(1)-C(2) bond length is 1.40 Å. The C(1)-N(1) bond length is 1.33 Å. The C(1)-H(1) bond length is 0.93 Å. In the second C site, C(2) is bonded in a distorted bent 120 degrees geometry to one C(1), one N(2), and one H(2) atom. The C(2)-N(2) bond length is 1.32 Å. The C(2)-H(2) bond length is 0.93 Å. In the third C site, C(3) is bonded in a distorted single-bond geometry to one N(2) atom. The C(3)-N(2) bond length is 1.35 Å. In the fourth C site, C(4) is bonded in a distorted single-bond geometry to one N(1) atom. The C(4)-N(1) bond length is 1.36 Å. There are two inequivalent N sites. In the first N site, N(1) is bonded in a trigonal planar geometry to one Cu(1), one C(1), and one C(4) atom. In the second N site, N(2) is bonded in a trigonal planar geometry to one Cu(1), one C(2), and one C(3) atom. There are two inequivalent H sites. In the first H site, H(1) is bonded in a single-bond geometry to one C(1) atom. In the second H site, H(2) is bonded in a single-bond geometry to one C(2) atom. Linkers: 4 c1cnc2c(n1)c1nccnc1c1nccnc21. Metal clusters: 4 [Cu]. The MOF has largest included sphere 5.01 A, density 1.17 g/cm3, surface area 3771.21 m2/g, accessible volume 0.45 cm3/g