Rb2Mo2C5P2H8S2(NO5)2 crystallizes in the tetragonal P4_2/n space group. There are two inequivalent Rb sites. In the first Rb site, Rb(1) is bonded in a 6-coordinate geometry to one S(1), one S(2), two equivalent O(1), and two equivalent O(5) atoms. The Rb(1)-S(1) bond length is 3.67 Å. The Rb(1)-S(2) bond length is 3.54 Å. There is one shorter (3.04 Å) and one longer (3.11 Å) Rb(1)-O(1) bond length. There is one shorter (3.10 Å) and one longer (3.12 Å) Rb(1)-O(5) bond length. In the second Rb site, Rb(2) is bonded in a 2-coordinate geometry to one S(1), one S(2), one O(3), and one O(8) atom. The Rb(2)-S(1) bond length is 3.56 Å. The Rb(2)-S(2) bond length is 3.59 Å. The Rb(2)-O(3) bond length is 2.88 Å. The Rb(2)-O(8) bond length is 3.00 Å. There are two inequivalent Mo sites. In the first Mo site, Mo(1) is bonded in a 6-coordinate geometry to one S(1), one S(2), one O(1), one O(2), one O(3), and one O(4) atom. The Mo(1)-S(1) bond length is 2.32 Å. The Mo(1)-S(2) bond length is 2.32 Å. The Mo(1)-O(1) bond length is 1.69 Å. The Mo(1)-O(2) bond length is 2.07 Å. The Mo(1)-O(3) bond length is 2.11 Å. The Mo(1)-O(4) bond length is 2.39 Å. In the second Mo site, Mo(2) is bonded in a 6-coordinate geometry to one S(1), one S(2), one O(5), one O(6), one O(7), and one O(8) atom. The Mo(2)-S(1) bond length is 2.32 Å. The Mo(2)-S(2) bond length is 2.33 Å. The Mo(2)-O(5) bond length is 1.68 Å. The Mo(2)-O(6) bond length is 2.10 Å. The Mo(2)-O(7) bond length is 2.11 Å. The Mo(2)-O(8) bond length is 2.40 Å. There are five inequivalent C sites. In the first C site, C(1) is bonded in a 4-coordinate geometry to one C(2), one P(1), one P(2), and one O(2) atom. The C(1)-C(2) bond length is 1.53 Å. The C(1)-P(1) bond length is 1.83 Å. The C(1)-P(2) bond length is 1.84 Å. The C(1)-O(2) bond length is 1.43 Å. In the second C site, C(2) is bonded in a 3-coordinate geometry to one C(1); one N(1); and two equivalent H(3,4) atoms. The C(2)-N(1) bond length is 1.47 Å. Both C(2)-H(3,4) bond lengths are 0.99 Å. In the third C site, C(3) is bonded in a 3-coordinate geometry to one C(4), one N(1), and one H(5) atom. The C(3)-C(4) bond length is 1.35 Å. The C(3)-N(1) bond length is 1.38 Å. The C(3)-H(5) bond length is 0.95 Å. In the fourth C site, C(4) is bonded in a 2-coordinate geometry to one C(3), one N(2), and one H(6) atom. The C(4)-N(2) bond length is 1.36 Å. The C(4)-H(6) bond length is 0.95 Å. In the fifth C site, C(5) is bonded in a trigonal planar geometry to one N(1), one N(2), and one H(7) atom. The C(5)-N(1) bond length is 1.32 Å. The C(5)-N(2) bond length is 1.32 Å. The C(5)-H(7) bond length is 0.95 Å. There are two inequivalent P sites. In the first P site, P(1) is bonded to one C(1), one O(4), one O(6), and one O(9) atom to form corner-sharing PCO3 tetrahedra. The P(1)-O(4) bond length is 1.53 Å. The P(1)-O(6) bond length is 1.54 Å. The P(1)-O(9) bond length is 1.51 Å. In the second P site, P(2) is bonded to one C(1), one O(10), one O(3), and one O(7) atom to form corner-sharing PCO3 tetrahedra. The P(2)-O(10) bond length is 1.50 Å. The P(2)-O(3) bond length is 1.54 Å. The P(2)-O(7) bond length is 1.54 Å. There are two inequivalent N sites. In the first N site, N(1) is bonded in a trigonal planar geometry to one C(2), one C(3), and one C(5) atom. In the second N site, N(2) is bonded in a trigonal planar geometry to one C(4), one C(5), and one H(8) atom. The N(2)-H(8) bond length is 0.88 Å. There are seven inequivalent H sites. In the first H site, H(1) is bonded in a single-bond geometry to one O(8) atom. The H(1)-O(8) bond length is 0.81 Å. In the second H site, H(2) is bonded in a single-bond geometry to one O(8) atom. The H(2)-O(8) bond length is 0.70 Å. In the third H site, H(3,4) is bonded in a single-bond geometry to one C(2) atom. In the fourth H site, H(5) is bonded in a single-bond geometry to one C(3) atom. In the fifth H site, H(6) is bonded in a single-bond geometry to one C(4) atom. In the sixth H site, H(7) is bonded in a single-bond geometry to one C(5) atom. In the seventh H site, H(8) is bonded in a single-bond geometry to one N(2) atom. There are two inequivalent S sites. In the first S site, S(1) is bonded in a 4-coordinate geometry to one Rb(1), one Rb(2), one Mo(1), and one Mo(2) atom. In the second S site, S(2) is bonded in a distorted rectangular see-saw-like geometry to one Rb(1), one Rb(2), one Mo(1), and one Mo(2) atom. There are ten inequivalent O sites. In the first O site, O(1) is bonded in a distorted single-bond geometry to two equivalent Rb(1) and one Mo(1) atom. In the second O site, O(2) is bonded in a distorted bent 120 degrees geometry to one Mo(1) and one C(1) atom. In the third O site, O(3) is bonded in a 3-coordinate geometry to one Rb(2), one Mo(1), and one P(2) atom. In the fourth O site, O(4) is bonded in a distorted single-bond geometry to one Mo(1) and one P(1) atom. In the fifth O site, O(5) is bonded in a single-bond geometry to two equivalent Rb(1) and one Mo(2) atom. In the sixth O site, O(6) is bonded in a distorted bent 150 degrees geometry to one Mo(2) and one P(1) atom. In the seventh O site, O(7) is bonded in a distorted bent 150 degrees geometry to one Mo(2) and one P(2) atom. In the eighth O site, O(8) is bonded in a water-like geometry to one Rb(2), one Mo(2), one H(1), and one H(2) atom. In the ninth O site, O(9) is bonded in a single-bond geometry to one P(1) atom. In the tenth O site, O(10) is bonded in a single-bond geometry to one P(2) atom. Linkers: 8 [O]C(CN1[CH]NC=C1)(P([O])([O])=O)P([O])([O])=O. Metal clusters: 16 [Rb] ,16 [Mo]. The MOF has largest included sphere 6.13 A, density 1.87 g/cm3, surface area 2733.05 m2/g, accessible volume 0.25 cm3/g