Ni2C28N2H22O11(C4NH3)2 crystallizes in the monoclinic C2/c space group. The structure consists of four C4NH3 clusters inside a Ni2C28N2H22O11 framework. In each C4NH3 cluster, there are four inequivalent C sites. In the first C site, C(14) is bonded in a distorted bent 120 degrees geometry to one C(2), one N(2), and one H(10) atom. The C(14)-C(2) bond length is 1.46 Å. The C(14)-N(2) bond length is 1.30 Å. The C(14)-H(10) bond length is 1.10 Å. In the second C site, C(15) is bonded in a distorted single-bond geometry to one C(2) and one H(11) atom. The C(15)-C(2) bond length is 1.41 Å. The C(15)-H(11) bond length is 1.09 Å. In the third C site, C(16) is bonded in a distorted single-bond geometry to one C(2) and one H(12) atom. The C(16)-C(2) bond length is 1.40 Å. The C(16)-H(12) bond length is 1.09 Å. In the fourth C site, C(2) is bonded in a trigonal planar geometry to one C(14), one C(15), and one C(16) atom. N(2) is bonded in a distorted water-like geometry to one C(14) and one N(2) atom. The N(2)-N(2) bond length is 1.40 Å. There are three inequivalent H sites. In the first H site, H(10) is bonded in a single-bond geometry to one C(14) atom. In the second H site, H(11) is bonded in a single-bond geometry to one C(15) atom. In the third H site, H(12) is bonded in a single-bond geometry to one C(16) atom. In the Ni2C28N2H22O11 framework, Ni(1) is bonded to one N(1), one O(1), one O(2), one O(3), one O(4), and one O(5) atom to form corner-sharing NiNO5 octahedra. The corner-sharing octahedral tilt angles are 64°. The Ni(1)-N(1) bond length is 2.05 Å. The Ni(1)-O(1) bond length is 2.06 Å. The Ni(1)-O(2) bond length is 2.26 Å. The Ni(1)-O(3) bond length is 2.02 Å. The Ni(1)-O(4) bond length is 2.03 Å. The Ni(1)-O(5) bond length is 2.06 Å. There are fourteen inequivalent C sites. In the first C site, C(3) is bonded in a trigonal planar geometry to one C(4), one C(5), and one C(8) atom. The C(3)-C(4) bond length is 1.38 Å. The C(3)-C(5) bond length is 1.50 Å. The C(3)-C(8) bond length is 1.42 Å. In the second C site, C(4) is bonded in a distorted single-bond geometry to one C(3), one C(6), and one H(4) atom. The C(4)-C(6) bond length is 1.41 Å. The C(4)-H(4) bond length is 1.09 Å. In the third C site, C(5) is bonded in a distorted bent 120 degrees geometry to one C(3), one O(4), and one O(5) atom. The C(5)-O(4) bond length is 1.28 Å. The C(5)-O(5) bond length is 1.27 Å. In the fourth C site, C(6) is bonded in a trigonal planar geometry to one C(17), one C(4), and one C(6) atom. The C(6)-C(17) bond length is 1.42 Å. The C(6)-C(6) bond length is 1.43 Å. In the fifth C site, C(7) is bonded in a distorted single-bond geometry to one C(1), one C(11), and one H(5) atom. The C(7)-C(1) bond length is 1.41 Å. The C(7)-C(11) bond length is 1.38 Å. The C(7)-H(5) bond length is 1.09 Å. In the sixth C site, C(8) is bonded in a distorted single-bond geometry to one C(3) and one H(6) atom. The C(8)-H(6) bond length is 1.09 Å. In the seventh C site, C(9) is bonded in a distorted single-bond geometry to one C(11) and one H(7) atom. The C(9)-C(11) bond length is 1.42 Å. The C(9)-H(7) bond length is 1.09 Å. In the eighth C site, C(10) is bonded in a distorted bent 120 degrees geometry to one N(1) and one H(8) atom. The C(10)-N(1) bond length is 1.34 Å. The C(10)-H(8) bond length is 1.09 Å. In the ninth C site, C(11) is bonded in a trigonal planar geometry to one C(12), one C(7), and one C(9) atom. The C(11)-C(12) bond length is 1.49 Å. In the tenth C site, C(12) is bonded in a distorted bent 120 degrees geometry to one C(11), one O(3), and one O(6) atom. The C(12)-O(3) bond length is 1.28 Å. The C(12)-O(6) bond length is 1.27 Å. In the eleventh C site, C(13) is bonded in a distorted single-bond geometry to one C(1) and one H(9) atom. The C(13)-C(1) bond length is 1.42 Å. The C(13)-H(9) bond length is 1.09 Å. In the twelfth C site, C(17) is bonded in a distorted single-bond geometry to one C(6) and one H(13) atom. The C(17)-H(13) bond length is 1.09 Å. In the thirteenth C site, C(18) is bonded in a distorted bent 120 degrees geometry to one N(1) and one H(14) atom. The C(18)-N(1) bond length is 1.35 Å. The C(18)-H(14) bond length is 1.09 Å. In the fourteenth C site, C(1) is bonded in a trigonal planar geometry to one C(1), one C(13), and one C(7) atom. The C(1)-C(1) bond length is 1.43 Å. N(1) is bonded in a trigonal planar geometry to one Ni(1), one C(10), and one C(18) atom. There are eleven inequivalent H sites. In the first H site, H(1) is bonded in a distorted single-bond geometry to one O(1) and one O(6) atom. The H(1)-O(1) bond length is 1.05 Å. The H(1)-O(6) bond length is 1.45 Å. In the second H site, H(2) is bonded in a single-bond geometry to one O(2) atom. The H(2)-O(2) bond length is 0.99 Å. In the third H site, H(3) is bonded in a single-bond geometry to one O(2) atom. The H(3)-O(2) bond length is 0.98 Å. In the fourth H site, H(4) is bonded in a single-bond geometry to one C(4) atom. In the fifth H site, H(5) is bonded in a single-bond geometry to one C(7) atom. In the sixth H site, H(6) is bonded in a single-bond geometry to one C(8) atom. In the seventh H site, H(7) is bonded in a single-bond geometry to one C(9) atom. In the eighth H site, H(8) is bonded in a single-bond geometry to one C(10) atom. In the ninth H site, H(9) is bonded in a single-bond geometry to one C(13) atom. In the tenth H site, H(13) is bonded in a single-bond geometry to one C(17) atom. In the eleventh H site, H(14) is bonded in a single-bond geometry to one C(18) atom. There are six inequivalent O sites. In the first O site, O(1) is bonded in a distorted water-like geometry to two equivalent Ni(1) and two equivalent H(1) atoms. In the second O site, O(2) is bonded in a distorted water-like geometry to one Ni(1), one H(2), and one H(3) atom. In the third O site, O(3) is bonded in a bent 120 degrees geometry to one Ni(1) and one C(12) atom. In the fourth O site, O(4) is bonded in a distorted bent 120 degrees geometry to one Ni(1) and one C(5) atom. In the fifth O site, O(5) is bonded in a distorted bent 120 degrees geometry to one Ni(1) and one C(5) atom. In the sixth O site, O(6) is bonded in a water-like geometry to one C(12) and one H(1) atom. Linkers: 4 [O]C(=O)c1ccc2cc(C([O])=O)ccc2c1 ,2 [CH]([N][N][CH]c1ccncc1)c1ccncc1. Metal clusters: 2 O.O.O.O=[C]O[Ni]1O[C]O[Ni](O[C]=O)O[C]O1. RCSR code: dia. The MOF has largest included sphere 5.52 A, density 1.23 g/cm3, surface area 4290.37 m2/g, accessible volume 0.26 cm3/g