Mo6Ni4CN crystallizes in the orthorhombic C222_1 space group. There are four inequivalent Mo sites. In the first Mo site, Mo(1) is bonded in a distorted bent 150 degrees geometry to three equivalent Ni(1), three equivalent Ni(2), one C(1), and one N(1) atom. In the second Mo site, Mo(2) is bonded in a distorted bent 150 degrees geometry to three equivalent Ni(1), three equivalent Ni(2), one C(1), and one N(1) atom. In the third Mo site, Mo(3) is bonded in a bent 150 degrees geometry to two equivalent Ni(2), four equivalent Ni(1), and two equivalent N(1) atoms. In the fourth Mo site, Mo(4) is bonded in a distorted bent 150 degrees geometry to two equivalent Ni(1), four equivalent Ni(2), and two equivalent C(1) atoms. There are two inequivalent Ni sites. In the first Ni site, Ni(1) is bonded to one Mo(4), two equivalent Mo(3), three equivalent Mo(1), three equivalent Mo(2), one Ni(1), and two equivalent Ni(2) atoms to form NiNi3Mo9 cuboctahedra that share corners with seven equivalent Ni(1)Ni3Mo9 cuboctahedra, corners with eight equivalent Ni(2)Ni3Mo9 cuboctahedra,  an edgeedge with one C(1)Mo6 octahedra, edges with two equivalent N(1)Mo6 octahedra, faces with four equivalent Ni(1)Ni3Mo9 cuboctahedra, faces with six equivalent Ni(2)Ni3Mo9 cuboctahedra, faces with two equivalent C(1)Mo6 octahedra, and faces with two equivalent N(1)Mo6 octahedra. In the second Ni site, Ni(2) is bonded to one Mo(3), two equivalent Mo(4), three equivalent Mo(1), three equivalent Mo(2), one Ni(2), and two equivalent Ni(1) atoms to form NiNi3Mo9 cuboctahedra that share corners with seven equivalent Ni(2)Ni3Mo9 cuboctahedra, corners with eight equivalent Ni(1)Ni3Mo9 cuboctahedra,  an edgeedge with one N(1)Mo6 octahedra, edges with two equivalent C(1)Mo6 octahedra, faces with four equivalent Ni(2)Ni3Mo9 cuboctahedra, faces with six equivalent Ni(1)Ni3Mo9 cuboctahedra, faces with two equivalent C(1)Mo6 octahedra, and faces with two equivalent N(1)Mo6 octahedra. C(1) is bonded to two equivalent Mo(1), two equivalent Mo(2), and two equivalent Mo(4) atoms to form distorted CMo6 octahedra that share corners with two equivalent C(1)Mo6 octahedra, corners with four equivalent N(1)Mo6 octahedra, edges with two equivalent Ni(1)Ni3Mo9 cuboctahedra, edges with four equivalent Ni(2)Ni3Mo9 cuboctahedra, faces with four equivalent Ni(1)Ni3Mo9 cuboctahedra, and faces with four equivalent Ni(2)Ni3Mo9 cuboctahedra. The corner-sharing octahedral tilt angles range from 25-26°. N(1) is bonded to two equivalent Mo(1), two equivalent Mo(2), and two equivalent Mo(3) atoms to form distorted NMo6 octahedra that share corners with two equivalent N(1)Mo6 octahedra, corners with four equivalent C(1)Mo6 octahedra, edges with two equivalent Ni(2)Ni3Mo9 cuboctahedra, edges with four equivalent Ni(1)Ni3Mo9 cuboctahedra, faces with four equivalent Ni(1)Ni3Mo9 cuboctahedra, and faces with four equivalent Ni(2)Ni3Mo9 cuboctahedra. The corner-sharing octahedral tilt angles range from 25-26°.
Mo6Ni4CN crystallizes in the orthorhombic C222_1 space group. There are four inequivalent Mo sites. In the first Mo site, Mo(1) is bonded in a distorted bent 150 degrees geometry to three equivalent Ni(1), three equivalent Ni(2), one C(1), and one N(1) atom. There are a spread of Mo(1)-Ni(1) bond distances ranging from 2.73-2.85 Å. There are a spread of Mo(1)-Ni(2) bond distances ranging from 2.74-2.78 Å. The Mo(1)-C(1) bond length is 2.10 Å. The Mo(1)-N(1) bond length is 2.11 Å. In the second Mo site, Mo(2) is bonded in a distorted bent 150 degrees geometry to three equivalent Ni(1), three equivalent Ni(2), one C(1), and one N(1) atom. There are a spread of Mo(2)-Ni(1) bond distances ranging from 2.73-2.78 Å. There are a spread of Mo(2)-Ni(2) bond distances ranging from 2.73-2.84 Å. The Mo(2)-C(1) bond length is 2.09 Å. The Mo(2)-N(1) bond length is 2.10 Å. In the third Mo site, Mo(3) is bonded in a bent 150 degrees geometry to two equivalent Ni(2), four equivalent Ni(1), and two equivalent N(1) atoms. Both Mo(3)-Ni(2) bond lengths are 2.75 Å. There are two shorter (2.77 Å) and two longer (2.84 Å) Mo(3)-Ni(1) bond lengths. Both Mo(3)-N(1) bond lengths are 2.09 Å. In the fourth Mo site, Mo(4) is bonded in a distorted bent 150 degrees geometry to two equivalent Ni(1), four equivalent Ni(2), and two equivalent C(1) atoms. Both Mo(4)-Ni(1) bond lengths are 2.72 Å. There are two shorter (2.78 Å) and two longer (2.84 Å) Mo(4)-Ni(2) bond lengths. Both Mo(4)-C(1) bond lengths are 2.11 Å. There are two inequivalent Ni sites. In the first Ni site, Ni(1) is bonded to one Mo(4), two equivalent Mo(3), three equivalent Mo(1), three equivalent Mo(2), one Ni(1), and two equivalent Ni(2) atoms to form NiNi3Mo9 cuboctahedra that share corners with seven equivalent Ni(1)Ni3Mo9 cuboctahedra, corners with eight equivalent Ni(2)Ni3Mo9 cuboctahedra,  an edgeedge with one C(1)Mo6 octahedra, edges with two equivalent N(1)Mo6 octahedra, faces with four equivalent Ni(1)Ni3Mo9 cuboctahedra, faces with six equivalent Ni(2)Ni3Mo9 cuboctahedra, faces with two equivalent C(1)Mo6 octahedra, and faces with two equivalent N(1)Mo6 octahedra. The Ni(1)-Ni(1) bond length is 2.48 Å. There is one shorter (2.48 Å) and one longer (2.49 Å) Ni(1)-Ni(2) bond length. In the second Ni site, Ni(2) is bonded to one Mo(3), two equivalent Mo(4), three equivalent Mo(1), three equivalent Mo(2), one Ni(2), and two equivalent Ni(1) atoms to form NiNi3Mo9 cuboctahedra that share corners with seven equivalent Ni(2)Ni3Mo9 cuboctahedra, corners with eight equivalent Ni(1)Ni3Mo9 cuboctahedra,  an edgeedge with one N(1)Mo6 octahedra, edges with two equivalent C(1)Mo6 octahedra, faces with four equivalent Ni(2)Ni3Mo9 cuboctahedra, faces with six equivalent Ni(1)Ni3Mo9 cuboctahedra, faces with two equivalent C(1)Mo6 octahedra, and faces with two equivalent N(1)Mo6 octahedra. The Ni(2)-Ni(2) bond length is 2.48 Å. C(1) is bonded to two equivalent Mo(1), two equivalent Mo(2), and two equivalent Mo(4) atoms to form distorted CMo6 octahedra that share corners with two equivalent C(1)Mo6 octahedra, corners with four equivalent N(1)Mo6 octahedra, edges with two equivalent Ni(1)Ni3Mo9 cuboctahedra, edges with four equivalent Ni(2)Ni3Mo9 cuboctahedra, faces with four equivalent Ni(1)Ni3Mo9 cuboctahedra, and faces with four equivalent Ni(2)Ni3Mo9 cuboctahedra. The corner-sharing octahedral tilt angles range from 25-26°. N(1) is bonded to two equivalent Mo(1), two equivalent Mo(2), and two equivalent Mo(3) atoms to form distorted NMo6 octahedra that share corners with two equivalent N(1)Mo6 octahedra, corners with four equivalent C(1)Mo6 octahedra, edges with two equivalent Ni(2)Ni3Mo9 cuboctahedra, edges with four equivalent Ni(1)Ni3Mo9 cuboctahedra, faces with four equivalent Ni(1)Ni3Mo9 cuboctahedra, and faces with four equivalent Ni(2)Ni3Mo9 cuboctahedra. The corner-sharing octahedral tilt angles range from 25-26°.