NiH12(CN)10 crystallizes in the triclinic P-1 space group. There are two inequivalent Ni sites. In the first Ni site, Ni(1) is bonded to two equivalent N(1), two equivalent N(5), and two equivalent N(8) atoms to form NiN6 octahedra that share corners with two equivalent C(1)H2N2 tetrahedra, corners with two equivalent C(4)H2N2 tetrahedra, and corners with two equivalent C(5)H2N2 tetrahedra. Both Ni(1)-N(1) bond lengths are 2.26 Å. Both Ni(1)-N(5) bond lengths are 2.03 Å. Both Ni(1)-N(8) bond lengths are 2.02 Å. In the second Ni site, Ni(2) is bonded to two equivalent N(10), two equivalent N(2), and two equivalent N(7) atoms to form NiN6 octahedra that share corners with two equivalent C(1)H2N2 tetrahedra, corners with two equivalent C(2)H2N2 tetrahedra, and corners with two equivalent C(6)H2N2 tetrahedra. Both Ni(2)-N(10) bond lengths are 2.02 Å. Both Ni(2)-N(2) bond lengths are 2.26 Å. Both Ni(2)-N(7) bond lengths are 2.03 Å. There are ten inequivalent C sites. In the first C site, C(1) is bonded to one N(1), one N(2), one H(1), and one H(2) atom to form CH2N2 tetrahedra that share  a cornercorner with one Ni(1)N6 octahedra,  a cornercorner with one Ni(2)N6 octahedra,  a cornercorner with one C(2)H2N2 tetrahedra,  a cornercorner with one C(4)H2N2 tetrahedra,  a cornercorner with one C(5)H2N2 tetrahedra, and  a cornercorner with one C(6)H2N2 tetrahedra. The corner-sharing octahedral tilt angles range from 72-73°. The C(1)-N(1) bond length is 1.48 Å. The C(1)-N(2) bond length is 1.48 Å. The C(1)-H(1) bond length is 1.09 Å. The C(1)-H(2) bond length is 1.09 Å. In the second C site, C(2) is bonded to one N(2), one N(3), one H(3), and one H(4) atom to form CH2N2 tetrahedra that share  a cornercorner with one Ni(2)N6 octahedra,  a cornercorner with one C(1)H2N2 tetrahedra,  a cornercorner with one C(3)H2N2 tetrahedra,  a cornercorner with one C(5)H2N2 tetrahedra, and  a cornercorner with one C(6)H2N2 tetrahedra. The corner-sharing octahedral tilt angles are 69°. The C(2)-N(2) bond length is 1.49 Å. The C(2)-N(3) bond length is 1.46 Å. The C(2)-H(3) bond length is 1.10 Å. The C(2)-H(4) bond length is 1.10 Å. In the third C site, C(3) is bonded to one N(3), one N(4), one H(5), and one H(6) atom to form corner-sharing CH2N2 tetrahedra. The C(3)-N(3) bond length is 1.47 Å. The C(3)-N(4) bond length is 1.47 Å. The C(3)-H(5) bond length is 1.10 Å. The C(3)-H(6) bond length is 1.10 Å. In the fourth C site, C(4) is bonded to one N(1), one N(4), one H(7), and one H(8) atom to form CH2N2 tetrahedra that share  a cornercorner with one Ni(1)N6 octahedra,  a cornercorner with one C(1)H2N2 tetrahedra,  a cornercorner with one C(3)H2N2 tetrahedra,  a cornercorner with one C(5)H2N2 tetrahedra, and  a cornercorner with one C(6)H2N2 tetrahedra. The corner-sharing octahedral tilt angles are 69°. The C(4)-N(1) bond length is 1.49 Å. The C(4)-N(4) bond length is 1.46 Å. The C(4)-H(7) bond length is 1.10 Å. The C(4)-H(8) bond length is 1.10 Å. In the fifth C site, C(5) is bonded to one N(1), one N(3), one H(10), and one H(9) atom to form CH2N2 tetrahedra that share  a cornercorner with one Ni(1)N6 octahedra,  a cornercorner with one C(1)H2N2 tetrahedra,  a cornercorner with one C(2)H2N2 tetrahedra,  a cornercorner with one C(3)H2N2 tetrahedra, and  a cornercorner with one C(4)H2N2 tetrahedra. The corner-sharing octahedral tilt angles are 66°. The C(5)-N(1) bond length is 1.49 Å. The C(5)-N(3) bond length is 1.46 Å. The C(5)-H(10) bond length is 1.10 Å. The C(5)-H(9) bond length is 1.10 Å. In the sixth C site, C(6) is bonded to one N(2), one N(4), one H(11), and one H(12) atom to form CH2N2 tetrahedra that share  a cornercorner with one Ni(2)N6 octahedra,  a cornercorner with one C(1)H2N2 tetrahedra,  a cornercorner with one C(2)H2N2 tetrahedra,  a cornercorner with one C(3)H2N2 tetrahedra, and  a cornercorner with one C(4)H2N2 tetrahedra. The corner-sharing octahedral tilt angles are 65°. The C(6)-N(2) bond length is 1.49 Å. The C(6)-N(4) bond length is 1.46 Å. The C(6)-H(11) bond length is 1.10 Å. The C(6)-H(12) bond length is 1.10 Å. In the seventh C site, C(7) is bonded in a linear geometry to one N(5) and one N(6) atom. The C(7)-N(5) bond length is 1.18 Å. The C(7)-N(6) bond length is 1.30 Å. In the eighth C site, C(8) is bonded in a linear geometry to one N(6) and one N(7) atom. The C(8)-N(6) bond length is 1.30 Å. The C(8)-N(7) bond length is 1.18 Å. In the ninth C site, C(9) is bonded in a linear geometry to one N(8) and one N(9) atom. The C(9)-N(8) bond length is 1.18 Å. The C(9)-N(9) bond length is 1.30 Å. In the tenth C site, C(10) is bonded in a linear geometry to one N(10) and one N(9) atom. The C(10)-N(10) bond length is 1.18 Å. The C(10)-N(9) bond length is 1.29 Å. There are ten inequivalent N sites. In the first N site, N(1) is bonded to one Ni(1), one C(1), one C(4), and one C(5) atom to form corner-sharing NNiC3 tetrahedra. In the second N site, N(2) is bonded to one Ni(2), one C(1), one C(2), and one C(6) atom to form corner-sharing NNiC3 tetrahedra. In the third N site, N(3) is bonded in a trigonal non-coplanar geometry to one C(2), one C(3), and one C(5) atom. In the fourth N site, N(4) is bonded in a trigonal non-coplanar geometry to one C(3), one C(4), and one C(6) atom. In the fifth N site, N(5) is bonded in a linear geometry to one Ni(1) and one C(7) atom. In the sixth N site, N(6) is bonded in a bent 120 degrees geometry to one C(7) and one C(8) atom. In the seventh N site, N(7) is bonded in a distorted linear geometry to one Ni(2) and one C(8) atom. In the eighth N site, N(8) is bonded in a linear geometry to one Ni(1) and one C(9) atom. In the ninth N site, N(9) is bonded in a bent 120 degrees geometry to one C(10) and one C(9) atom. In the tenth N site, N(10) is bonded in a linear geometry to one Ni(2) and one C(10) atom. There are twelve 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 C(2) atom. In the fourth H site, H(4) is bonded in a single-bond geometry to one C(2) 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(3) atom. In the seventh H site, H(7) is bonded in a single-bond geometry to one C(4) atom. In the eighth H site, H(8) is bonded in a single-bond geometry to one C(4) atom. In the ninth H site, H(9) is bonded in a single-bond geometry to one C(5) atom. In the tenth H site, H(10) is bonded in a single-bond geometry to one C(5) atom. In the eleventh H site, H(11) is bonded in a single-bond geometry to one C(6) atom. In the twelfth H site, H(12) is bonded in a single-bond geometry to one C(6) atom. Linkers: 2 C1N2CN3CN1CN(C2)C3. Metal clusters: 2 [Ni]. The MOF has largest included sphere 3.07 A, density 1.58 g/cm3, surface area 3894.96 m2/g, accessible volume 0.09 cm3/g