AgCN4H crystallizes in the monoclinic P2_1/c space group. There are two inequivalent Ag sites. In the first Ag site, Ag(1) is bonded in a tetrahedral geometry to one N(2), one N(4), one N(7), and one N(8) atom. The Ag(1)-N(2) bond length is 2.29 Å. The Ag(1)-N(4) bond length is 2.37 Å. The Ag(1)-N(7) bond length is 2.37 Å. The Ag(1)-N(8) bond length is 2.25 Å. In the second Ag site, Ag(2) is bonded in a distorted trigonal planar geometry to one N(1), one N(5), and one N(6) atom. The Ag(2)-N(1) bond length is 2.18 Å. The Ag(2)-N(5) bond length is 2.19 Å. The Ag(2)-N(6) bond length is 2.34 Å. There are two inequivalent C sites. In the first C site, C(1) is bonded in a trigonal planar geometry to one N(1), one N(4), and one H(1) atom. The C(1)-N(1) bond length is 1.34 Å. The C(1)-N(4) bond length is 1.34 Å. The C(1)-H(1) bond length is 1.09 Å. In the second C site, C(2) is bonded in a trigonal planar geometry to one N(5), one N(8), and one H(2) atom. The C(2)-N(5) bond length is 1.34 Å. The C(2)-N(8) bond length is 1.34 Å. The C(2)-H(2) bond length is 1.08 Å. There are eight inequivalent N sites. In the first 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 1.32 Å. The N(3)-N(4) bond length is 1.35 Å. In the second N site, N(4) is bonded in a distorted single-bond geometry to one Ag(1), one C(1), and one N(3) atom. In the third N site, N(5) is bonded in a distorted trigonal planar geometry to one Ag(2), one C(2), and one N(6) atom. The N(5)-N(6) bond length is 1.35 Å. In the fourth N site, N(6) is bonded in a trigonal planar geometry to one Ag(2), one N(5), and one N(7) atom. The N(6)-N(7) bond length is 1.32 Å. In the fifth N site, N(7) is bonded in a trigonal planar geometry to one Ag(1), one N(6), and one N(8) atom. The N(7)-N(8) bond length is 1.35 Å. In the sixth N site, N(8) is bonded in a 3-coordinate geometry to one Ag(1), one C(2), and one N(7) atom. In the seventh N site, N(1) is bonded in a 3-coordinate geometry to one Ag(2), one C(1), and one N(2) atom. The N(1)-N(2) bond length is 1.35 Å. In the eighth N site, N(2) is bonded in a trigonal planar geometry to one Ag(1), one N(1), and one N(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: 8 C1=NN=N[N]1. Metal clusters: 8 [Ag]. The MOF has largest included sphere 1.77 A, density 3.36 g/cm3, surface area 2144.34 m2/g, accessible volume 0.06 cm3/g