Gd4Ni3C30H42(NO7)6 crystallizes in the triclinic P-1 space group. There are two inequivalent Gd sites. In the first Gd site, Gd(1) is bonded in a 9-coordinate geometry to one O(1), one O(14), one O(16), one O(17), one O(18), one O(19), one O(20), one O(3), and one O(4) atom. The Gd(1)-O(1) bond length is 2.28 Å. The Gd(1)-O(14) bond length is 2.48 Å. The Gd(1)-O(16) bond length is 2.48 Å. The Gd(1)-O(17) bond length is 2.58 Å. The Gd(1)-O(18) bond length is 2.43 Å. The Gd(1)-O(19) bond length is 2.44 Å. The Gd(1)-O(20) bond length is 2.44 Å. The Gd(1)-O(3) bond length is 2.61 Å. The Gd(1)-O(4) bond length is 2.48 Å. In the second Gd site, Gd(2) is bonded in a 9-coordinate geometry to one O(11), one O(12), one O(13), one O(15), one O(21), one O(6), one O(7), one O(8), and one O(9) atom. The Gd(2)-O(11) bond length is 2.47 Å. The Gd(2)-O(12) bond length is 2.65 Å. The Gd(2)-O(13) bond length is 2.46 Å. The Gd(2)-O(15) bond length is 2.50 Å. The Gd(2)-O(21) bond length is 2.38 Å. The Gd(2)-O(6) bond length is 2.30 Å. The Gd(2)-O(7) bond length is 2.57 Å. The Gd(2)-O(8) bond length is 2.53 Å. The Gd(2)-O(9) bond length is 2.28 Å. There are two inequivalent Ni sites. In the first Ni site, Ni(1) is bonded in an octahedral geometry to two equivalent N(2), two equivalent O(5), and two equivalent O(8) atoms. Both Ni(1)-N(2) bond lengths are 2.09 Å. Both Ni(1)-O(5) bond lengths are 2.06 Å. Both Ni(1)-O(8) bond lengths are 2.08 Å. In the second Ni site, Ni(2) is bonded in an octahedral geometry to one N(1), one N(3), one O(10), one O(11), one O(2), and one O(4) atom. The Ni(2)-N(1) bond length is 2.07 Å. The Ni(2)-N(3) bond length is 2.06 Å. The Ni(2)-O(10) bond length is 2.04 Å. The Ni(2)-O(11) bond length is 2.07 Å. The Ni(2)-O(2) bond length is 2.07 Å. The Ni(2)-O(4) bond length is 2.10 Å. There are fifteen inequivalent C sites. In the first C site, C(1) is bonded in a distorted trigonal non-coplanar geometry to one N(1), one H(1), and one H(2) atom. The C(1)-N(1) bond length is 1.47 Å. The C(1)-H(1) bond length is 1.10 Å. The C(1)-H(2) bond length is 1.10 Å. In the second C site, C(2) is bonded in a distorted bent 120 degrees geometry to one O(1) and one O(2) atom. The C(2)-O(1) bond length is 1.26 Å. The C(2)-O(2) bond length is 1.28 Å. In the third C site, C(3) is bonded in a distorted trigonal non-coplanar geometry to one N(1), one H(4), and one H(5) atom. The C(3)-N(1) bond length is 1.46 Å. The C(3)-H(4) bond length is 1.10 Å. The C(3)-H(5) bond length is 1.10 Å. In the fourth C site, C(4) is bonded in a distorted bent 120 degrees geometry to one O(3) and one O(4) atom. The C(4)-O(3) bond length is 1.25 Å. The C(4)-O(4) bond length is 1.30 Å. In the fifth C site, C(5) is bonded in a distorted trigonal non-coplanar geometry to one N(2), one H(6), and one H(7) atom. The C(5)-N(2) bond length is 1.48 Å. The C(5)-H(6) bond length is 1.10 Å. The C(5)-H(7) bond length is 1.10 Å. In the sixth C site, C(6) is bonded in a distorted bent 120 degrees geometry to one O(5) and one O(6) atom. The C(6)-O(5) bond length is 1.28 Å. The C(6)-O(6) bond length is 1.26 Å. In the seventh C site, C(7) is bonded in a distorted trigonal non-coplanar geometry to one N(2), one H(10), and one H(9) atom. The C(7)-N(2) bond length is 1.47 Å. The C(7)-H(10) bond length is 1.10 Å. The C(7)-H(9) bond length is 1.10 Å. In the eighth C site, C(8) is bonded in a distorted bent 120 degrees geometry to one O(7) and one O(8) atom. The C(8)-O(7) bond length is 1.26 Å. The C(8)-O(8) bond length is 1.29 Å. In the ninth C site, C(9) is bonded in a distorted trigonal non-coplanar geometry to one N(3), one H(11), and one H(12) atom. The C(9)-N(3) bond length is 1.48 Å. The C(9)-H(11) bond length is 1.10 Å. The C(9)-H(12) bond length is 1.10 Å. In the tenth C site, C(10) is bonded in a distorted bent 120 degrees geometry to one O(10) and one O(9) atom. The C(10)-O(10) bond length is 1.27 Å. The C(10)-O(9) bond length is 1.26 Å. In the eleventh C site, C(11) is bonded in a distorted trigonal non-coplanar geometry to one N(3), one H(14), and one H(15) atom. The C(11)-N(3) bond length is 1.47 Å. The C(11)-H(14) bond length is 1.10 Å. The C(11)-H(15) bond length is 1.10 Å. In the twelfth C site, C(12) is bonded in a distorted bent 120 degrees geometry to one O(11) and one O(12) atom. The C(12)-O(11) bond length is 1.29 Å. The C(12)-O(12) bond length is 1.26 Å. In the thirteenth C site, C(13) is bonded in a distorted bent 120 degrees geometry to one O(13) and one O(14) atom. The C(13)-O(13) bond length is 1.26 Å. The C(13)-O(14) bond length is 1.27 Å. In the fourteenth C site, C(14) is bonded in a distorted bent 120 degrees geometry to one O(15) and one O(16) atom. The C(14)-O(15) bond length is 1.27 Å. The C(14)-O(16) bond length is 1.26 Å. In the fifteenth C site, C(15) is bonded in a distorted bent 120 degrees geometry to one O(17) and one O(18) atom. The C(15)-O(17) bond length is 1.27 Å. The C(15)-O(18) bond length is 1.27 Å. There are three inequivalent N sites. In the first N site, N(1) is bonded to one Ni(2), one C(1), one C(3), and one H(3) atom to form distorted corner-sharing NNiHC2 tetrahedra. The N(1)-H(3) bond length is 1.03 Å. In the second N site, N(2) is bonded to one Ni(1), one C(5), one C(7), and one H(8) atom to form distorted corner-sharing NNiHC2 tetrahedra. The N(2)-H(8) bond length is 1.02 Å. In the third N site, N(3) is bonded to one Ni(2), one C(11), one C(9), and one H(13) atom to form distorted corner-sharing NNiHC2 tetrahedra. The N(3)-H(13) bond length is 1.02 Å. There are twenty-one 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(1) atom. In the third H site, H(3) is bonded in a single-bond geometry to one N(1) atom. In the fourth H site, H(4) is bonded in a single-bond geometry to one C(3) atom. In the fifth H site, H(5) is bonded in a single-bond geometry to one C(3) atom. In the sixth H site, H(6) is bonded in a single-bond geometry to one C(5) atom. In the seventh H site, H(7) is bonded in a single-bond geometry to one C(5) atom. In the eighth H site, H(8) is bonded in a single-bond geometry to one N(2) atom. In the ninth H site, H(9) is bonded in a single-bond geometry to one C(7) atom. In the tenth H site, H(10) is bonded in a single-bond geometry to one C(7) atom. In the eleventh H site, H(11) is bonded in a single-bond geometry to one C(9) atom. In the twelfth H site, H(12) is bonded in a single-bond geometry to one C(9) atom. In the thirteenth H site, H(13) is bonded in a single-bond geometry to one N(3) atom. In the fourteenth H site, H(14) is bonded in a single-bond geometry to one C(11) atom. In the fifteenth H site, H(15) is bonded in a single-bond geometry to one C(11) atom. In the sixteenth H site, H(16) is bonded in a single-bond geometry to one O(19) atom. The H(16)-O(19) bond length is 0.99 Å. In the seventeenth H site, H(17) is bonded in a single-bond geometry to one O(19) atom. The H(17)-O(19) bond length is 1.00 Å. In the eighteenth H site, H(18) is bonded in a distorted single-bond geometry to one O(15) and one O(20) atom. The H(18)-O(15) bond length is 1.69 Å. The H(18)-O(20) bond length is 1.00 Å. In the nineteenth H site, H(19) is bonded in a single-bond geometry to one O(20) atom. The H(19)-O(20) bond length is 0.99 Å. In the twentieth H site, H(20) is bonded in a linear geometry to one O(14) and one O(21) atom. The H(20)-O(14) bond length is 1.61 Å. The H(20)-O(21) bond length is 1.01 Å. In the twenty-first H site, H(21) is bonded in a single-bond geometry to one O(21) atom. The H(21)-O(21) bond length is 0.97 Å. There are twenty-one inequivalent O sites. In the first O site, O(1) is bonded in a distorted bent 150 degrees geometry to one Gd(1) and one C(2) atom. In the second O site, O(2) is bonded in a 2-coordinate geometry to one Ni(2) and one C(2) atom. In the third O site, O(3) is bonded in a single-bond geometry to one Gd(1) and one C(4) atom. In the fourth O site, O(4) is bonded in a 3-coordinate geometry to one Gd(1), one Ni(2), and one C(4) atom. In the fifth O site, O(5) is bonded in a bent 120 degrees geometry to one Ni(1) and one C(6) atom. In the sixth O site, O(6) is bonded in a bent 150 degrees geometry to one Gd(2) and one C(6) atom. In the seventh O site, O(7) is bonded in a distorted single-bond geometry to one Gd(2) and one C(8) atom. In the eighth O site, O(8) is bonded in a 3-coordinate geometry to one Gd(2), one Ni(1), and one C(8) atom. In the ninth O site, O(9) is bonded in a distorted bent 150 degrees geometry to one Gd(2) and one C(10) atom. In the tenth O site, O(10) is bonded in a bent 120 degrees geometry to one Ni(2) and one C(10) atom. In the eleventh O site, O(11) is bonded in a 3-coordinate geometry to one Gd(2), one Ni(2), and one C(12) atom. In the twelfth O site, O(12) is bonded in a single-bond geometry to one Gd(2) and one C(12) atom. In the thirteenth O site, O(13) is bonded in a distorted bent 120 degrees geometry to one Gd(2) and one C(13) atom. In the fourteenth O site, O(14) is bonded in a distorted trigonal planar geometry to one Gd(1), one C(13), and one H(20) atom. In the fifteenth O site, O(15) is bonded in a distorted trigonal planar geometry to one Gd(2), one C(14), and one H(18) atom. In the sixteenth O site, O(16) is bonded in a distorted single-bond geometry to one Gd(1) and one C(14) atom. In the seventeenth O site, O(17) is bonded in a single-bond geometry to one Gd(1) and one C(15) atom. In the eighteenth O site, O(18) is bonded in a distorted bent 120 degrees geometry to one Gd(1) and one C(15) atom. In the nineteenth O site, O(19) is bonded in a distorted water-like geometry to one Gd(1), one H(16), and one H(17) atom. In the twentieth O site, O(20) is bonded in a distorted water-like geometry to one Gd(1), one H(18), and one H(19) atom. In the twenty-first O site, O(21) is bonded in a distorted water-like geometry to one Gd(2), one H(20), and one H(21) atom. Linkers: 2 [O]C(=O)C([O])=O. Metal clusters: 4 [Gd] ,3 [Ni]. The MOF has largest included sphere 3.21 A, density 2.56 g/cm3, surface area 2452.88 m2/g, accessible volume 0.06 cm3/g