CrAl4S8 crystallizes in the cubic F-43m space group. Cr(1) is bonded to four equivalent S(1) atoms to form CrS4 tetrahedra that share corners with twelve equivalent Al(1)S6 octahedra. The corner-sharing octahedral tilt angles are 60°. Al(1) is bonded to three equivalent S(1) and three equivalent S(2) atoms to form AlS6 octahedra that share corners with three equivalent Cr(1)S4 tetrahedra and edges with six equivalent Al(1)S6 octahedra. There are two inequivalent S sites. In the first S site, S(1) is bonded to one Cr(1) and three equivalent Al(1) atoms to form a mixture of distorted corner and edge-sharing SAl3Cr tetrahedra. In the second S site, S(2) is bonded in a distorted T-shaped geometry to three equivalent Al(1) atoms.
CrAl4S8 crystallizes in the cubic F-43m space group. Cr(1) is bonded to four equivalent S(1) atoms to form CrS4 tetrahedra that share corners with twelve equivalent Al(1)S6 octahedra. The corner-sharing octahedral tilt angles are 60°. All Cr(1)-S(1) bond lengths are 2.21 Å. Al(1) is bonded to three equivalent S(1) and three equivalent S(2) atoms to form AlS6 octahedra that share corners with three equivalent Cr(1)S4 tetrahedra and edges with six equivalent Al(1)S6 octahedra. All Al(1)-S(1) bond lengths are 2.59 Å. All Al(1)-S(2) bond lengths are 2.32 Å. There are two inequivalent S sites. In the first S site, S(1) is bonded to one Cr(1) and three equivalent Al(1) atoms to form a mixture of distorted corner and edge-sharing SAl3Cr tetrahedra. In the second S site, S(2) is bonded in a distorted T-shaped geometry to three equivalent Al(1) atoms.