FeH4(C3N2)2 crystallizes in the orthorhombic Cccm space group. Fe(1) is bonded in a tetrahedral geometry to four equivalent N(1) atoms. All Fe(1)-N(1) bond lengths are 2.00 Å. There are two inequivalent C sites. In the first C site, C(1) is bonded in a trigonal planar geometry to one C(1) and two equivalent C(2) atoms. The C(1)-C(1) bond length is 1.45 Å. Both C(1)-C(2) bond lengths are 1.41 Å. In the second C site, C(2) is bonded in a distorted bent 120 degrees geometry to one C(1), one N(1), and one H(1) atom. The C(2)-N(1) bond length is 1.35 Å. The C(2)-H(1) bond length is 1.09 Å. N(1) is bonded in a distorted trigonal planar geometry to one Fe(1), one C(2), and one N(1) atom. The N(1)-N(1) bond length is 1.37 Å. H(1) is bonded in a single-bond geometry to one C(2) atom. Linkers: 1 [CH]1N=NC=C1[C]1C=NN=C1 ,1 C1=N[N]C=C1[C]1C=NN=C1. Metal clusters: 2 [Fe]. The MOF has largest included sphere 6.40 A, density 1.07 g/cm3, surface area 3788.63 m2/g, accessible volume 0.51 cm3/g