MoCu4C26H16(N7S2)2 crystallizes in the tetragonal I4_1/a space group. There are two inequivalent Mo sites. In the first Mo site, Mo(1) is bonded in a distorted tetrahedral geometry to four equivalent S(1) atoms. All Mo(1)-S(1) bond lengths are 2.23 Å. In the second Mo site, Mo(2) is bonded to four equivalent S(2) atoms to form distorted MoS4 tetrahedra that share edges with four equivalent Cu(2)CS2N tetrahedra. All Mo(2)-S(2) bond lengths are 2.23 Å. There are two inequivalent Cu sites. In the first Cu site, Cu(1) is bonded in a 4-coordinate geometry to one N(1), one N(2), and two equivalent S(1) atoms. The Cu(1)-N(1) bond length is 2.17 Å. The Cu(1)-N(2) bond length is 1.91 Å. There is one shorter (2.29 Å) and one longer (2.32 Å) Cu(1)-S(1) bond length. In the second Cu site, Cu(2) is bonded to one C(7), one N(5), and two equivalent S(2) atoms to form distorted CuCS2N tetrahedra that share corners with two equivalent Cu(2)CS2N tetrahedra and  an edgeedge with one Mo(2)S4 tetrahedra. The Cu(2)-C(7) bond length is 1.91 Å. The Cu(2)-N(5) bond length is 2.17 Å. There is one shorter (2.29 Å) and one longer (2.32 Å) Cu(2)-S(2) bond length. There are nine inequivalent C sites. In the first C site, C(1) is bonded in a distorted bent 120 degrees geometry to one N(1) and one H(1,5) atom. The C(1)-N(1) bond length is 1.32 Å. The C(1)-H(1,5) bond length is 0.93 Å. In the second C site, C(2,9) is bonded in a distorted single-bond geometry to one C(3,10) and one H(2,6) atom. The C(2,9)-C(3,10) bond length is 1.38 Å. The C(2,9)-H(2,6) bond length is 0.93 Å. In the third C site, C(3,10) is bonded in a trigonal planar geometry to one C(2,9); one C(4,11); and one C(6,13) atom. The C(3,10)-C(4,11) bond length is 1.35 Å. The C(3,10)-C(6,13) bond length is 1.48 Å. In the fourth C site, C(4,11) is bonded in a distorted trigonal planar geometry to one C(3,10); one C(5); and one H(3,7) atom. The C(4,11)-C(5) bond length is 1.39 Å. The C(4,11)-H(3,7) bond length is 0.93 Å. In the fifth C site, C(5) is bonded in a distorted bent 120 degrees geometry to one C(4,11); one N(1); and one H(4,8) atom. The C(5)-N(1) bond length is 1.31 Å. The C(5)-H(4,8) bond length is 0.93 Å. In the sixth C site, C(6,13) is bonded in a distorted trigonal planar geometry to one C(3,10); one N(3,6); and one N(4,7) atom. The C(6,13)-N(3,6) bond length is 1.33 Å. The C(6,13)-N(4,7) bond length is 1.32 Å. In the seventh C site, C(7) is bonded in a linear geometry to one Cu(2) and one N(2) atom. The C(7)-N(2) bond length is 1.15 Å. In the eighth C site, C(8) is bonded in a distorted bent 120 degrees geometry to one N(5) and one H(1,5) atom. The C(8)-N(5) bond length is 1.32 Å. The C(8)-H(1,5) bond length is 0.93 Å. In the ninth C site, C(12) is bonded in a distorted bent 120 degrees geometry to one C(4,11); one N(5); and one H(4,8) atom. The C(12)-C(4,11) bond length is 1.39 Å. The C(12)-N(5) bond length is 1.31 Å. The C(12)-H(4,8) bond length is 0.93 Å. There are five 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(5) atom. In the second N site, N(2) is bonded in a linear geometry to one Cu(1) and one C(7) atom. In the third N site, N(3,6) is bonded in a distorted bent 120 degrees geometry to one C(6,13) and one N(4,7) atom. The N(3,6)-N(4,7) bond length is 1.32 Å. In the fourth N site, N(4,7) is bonded in a distorted bent 120 degrees geometry to one C(6,13) and one N(3,6) atom. In the fifth N site, N(5) is bonded in a trigonal planar geometry to one Cu(2), one C(12), and one C(8) atom. There are four inequivalent H sites. In the first H site, H(1,5) is bonded in a single-bond geometry to one C(1) atom. In the second H site, H(2,6) is bonded in a single-bond geometry to one C(2,9) atom. In the third H site, H(3,7) is bonded in a single-bond geometry to one C(4,11) atom. In the fourth H site, H(4,8) is bonded in a single-bond geometry to one C(5) atom. There are two inequivalent S sites. In the first S site, S(1) is bonded in a distorted trigonal non-coplanar geometry to one Mo(1) and two equivalent Cu(1) atoms. In the second S site, S(2) is bonded in a distorted trigonal non-coplanar geometry to one Mo(2) and two equivalent Cu(2) atoms. Linkers: 12 c1cc(C2=N[N]C(c3ccncc3)=N[N]2)ccn1 ,3 c1cc(-c2nnc(-c3ccncc3)nn2)ccn1. Metal clusters: 32 [Cu] ,8 [Mo]. The MOF has largest included sphere 4.44 A, density 1.34 g/cm3, surface area 3794.32 m2/g, accessible volume 0.40 cm3/g