Cr(MoS2)2 crystallizes in the monoclinic C2/c space group. There are two inequivalent Mo sites. In the first Mo site, Mo(1) is bonded to one S(3), one S(4), two equivalent S(1), and two equivalent S(2) atoms to form distorted MoS6 octahedra that share corners with six equivalent Cr(1)S6 octahedra, edges with two equivalent Mo(1)S6 octahedra, edges with four equivalent Mo(2)S6 octahedra, and  a faceface with one Cr(1)S6 octahedra. The corner-sharing octahedral tilt angles range from 48-57°. In the second Mo site, Mo(2) is bonded to one S(1), one S(2), two equivalent S(3), and two equivalent S(4) atoms to form distorted MoS6 octahedra that share corners with six equivalent Cr(1)S6 octahedra, edges with two equivalent Mo(2)S6 octahedra, edges with four equivalent Mo(1)S6 octahedra, and  a faceface with one Cr(1)S6 octahedra. The corner-sharing octahedral tilt angles range from 48-59°. Cr(1) is bonded to one S(1), one S(4), two equivalent S(2), and two equivalent S(3) atoms to form CrS6 octahedra that share corners with six equivalent Mo(1)S6 octahedra, corners with six equivalent Mo(2)S6 octahedra, edges with two equivalent Cr(1)S6 octahedra,  a faceface with one Mo(1)S6 octahedra, and  a faceface with one Mo(2)S6 octahedra. The corner-sharing octahedral tilt angles range from 48-59°. There are four inequivalent S sites. In the first S site, S(3) is bonded in a 5-coordinate geometry to one Mo(1), two equivalent Mo(2), and two equivalent Cr(1) atoms. In the second S site, S(4) is bonded to one Mo(1), two equivalent Mo(2), and one Cr(1) atom to form distorted edge-sharing SCrMo3 trigonal pyramids. In the third S site, S(1) is bonded in a 4-coordinate geometry to one Mo(2), two equivalent Mo(1), and one Cr(1) atom. In the fourth S site, S(2) is bonded in a 5-coordinate geometry to one Mo(2), two equivalent Mo(1), and two equivalent Cr(1) atoms.
Cr(MoS2)2 crystallizes in the monoclinic C2/c space group. There are two inequivalent Mo sites. In the first Mo site, Mo(1) is bonded to one S(3), one S(4), two equivalent S(1), and two equivalent S(2) atoms to form distorted MoS6 octahedra that share corners with six equivalent Cr(1)S6 octahedra, edges with two equivalent Mo(1)S6 octahedra, edges with four equivalent Mo(2)S6 octahedra, and  a faceface with one Cr(1)S6 octahedra. The corner-sharing octahedral tilt angles range from 48-57°. The Mo(1)-S(3) bond length is 2.49 Å. The Mo(1)-S(4) bond length is 2.43 Å. There is one shorter (2.39 Å) and one longer (2.41 Å) Mo(1)-S(1) bond length. There is one shorter (2.57 Å) and one longer (2.61 Å) Mo(1)-S(2) bond length. In the second Mo site, Mo(2) is bonded to one S(1), one S(2), two equivalent S(3), and two equivalent S(4) atoms to form distorted MoS6 octahedra that share corners with six equivalent Cr(1)S6 octahedra, edges with two equivalent Mo(2)S6 octahedra, edges with four equivalent Mo(1)S6 octahedra, and  a faceface with one Cr(1)S6 octahedra. The corner-sharing octahedral tilt angles range from 48-59°. The Mo(2)-S(1) bond length is 2.38 Å. The Mo(2)-S(2) bond length is 2.59 Å. There is one shorter (2.49 Å) and one longer (2.63 Å) Mo(2)-S(3) bond length. There is one shorter (2.37 Å) and one longer (2.45 Å) Mo(2)-S(4) bond length. Cr(1) is bonded to one S(1), one S(4), two equivalent S(2), and two equivalent S(3) atoms to form CrS6 octahedra that share corners with six equivalent Mo(1)S6 octahedra, corners with six equivalent Mo(2)S6 octahedra, edges with two equivalent Cr(1)S6 octahedra,  a faceface with one Mo(1)S6 octahedra, and  a faceface with one Mo(2)S6 octahedra. The corner-sharing octahedral tilt angles range from 48-59°. The Cr(1)-S(1) bond length is 2.46 Å. The Cr(1)-S(4) bond length is 2.49 Å. Both Cr(1)-S(2) bond lengths are 2.51 Å. There is one shorter (2.47 Å) and one longer (2.50 Å) Cr(1)-S(3) bond length. There are four inequivalent S sites. In the first S site, S(3) is bonded in a 5-coordinate geometry to one Mo(1), two equivalent Mo(2), and two equivalent Cr(1) atoms. In the second S site, S(4) is bonded to one Mo(1), two equivalent Mo(2), and one Cr(1) atom to form distorted edge-sharing SCrMo3 trigonal pyramids. In the third S site, S(1) is bonded in a 4-coordinate geometry to one Mo(2), two equivalent Mo(1), and one Cr(1) atom. In the fourth S site, S(2) is bonded in a 5-coordinate geometry to one Mo(2), two equivalent Mo(1), and two equivalent Cr(1) atoms.