CrZnAlS4 is Spinel-derived structured and crystallizes in the orthorhombic Imma space group. Cr(1) is bonded to two equivalent S(2) and four equivalent S(1) atoms to form CrS6 octahedra that share corners with six equivalent Zn(1)S4 tetrahedra, edges with two equivalent Cr(1)S6 octahedra, and edges with four equivalent Al(1)S6 octahedra. Zn(1) is bonded to two equivalent S(1) and two equivalent S(2) atoms to form ZnS4 tetrahedra that share corners with six equivalent Cr(1)S6 octahedra and corners with six equivalent Al(1)S6 octahedra. The corner-sharing octahedral tilt angles are 58°. Al(1) is bonded to two equivalent S(1) and four equivalent S(2) atoms to form AlS6 octahedra that share corners with six equivalent Zn(1)S4 tetrahedra, edges with two equivalent Al(1)S6 octahedra, and edges with four equivalent Cr(1)S6 octahedra. There are two inequivalent S sites. In the first S site, S(1) is bonded to two equivalent Cr(1), one Zn(1), and one Al(1) atom to form distorted SAlZnCr2 trigonal pyramids that share corners with six equivalent S(2)Al2ZnCr trigonal pyramids, corners with six equivalent S(1)AlZnCr2 trigonal pyramids,  an edgeedge with one S(1)AlZnCr2 trigonal pyramid, and edges with two equivalent S(2)Al2ZnCr trigonal pyramids. In the second S site, S(2) is bonded to one Cr(1), one Zn(1), and two equivalent Al(1) atoms to form distorted SAl2ZnCr trigonal pyramids that share corners with six equivalent S(2)Al2ZnCr trigonal pyramids, corners with six equivalent S(1)AlZnCr2 trigonal pyramids,  an edgeedge with one S(2)Al2ZnCr trigonal pyramid, and edges with two equivalent S(1)AlZnCr2 trigonal pyramids.
CrZnAlS4 is Spinel-derived structured and crystallizes in the orthorhombic Imma space group. Cr(1) is bonded to two equivalent S(2) and four equivalent S(1) atoms to form CrS6 octahedra that share corners with six equivalent Zn(1)S4 tetrahedra, edges with two equivalent Cr(1)S6 octahedra, and edges with four equivalent Al(1)S6 octahedra. Both Cr(1)-S(2) bond lengths are 2.42 Å. All Cr(1)-S(1) bond lengths are 2.42 Å. Zn(1) is bonded to two equivalent S(1) and two equivalent S(2) atoms to form ZnS4 tetrahedra that share corners with six equivalent Cr(1)S6 octahedra and corners with six equivalent Al(1)S6 octahedra. The corner-sharing octahedral tilt angles are 58°. Both Zn(1)-S(1) bond lengths are 2.36 Å. Both Zn(1)-S(2) bond lengths are 2.35 Å. Al(1) is bonded to two equivalent S(1) and four equivalent S(2) atoms to form AlS6 octahedra that share corners with six equivalent Zn(1)S4 tetrahedra, edges with two equivalent Al(1)S6 octahedra, and edges with four equivalent Cr(1)S6 octahedra. Both Al(1)-S(1) bond lengths are 2.42 Å. All Al(1)-S(2) bond lengths are 2.42 Å. There are two inequivalent S sites. In the first S site, S(1) is bonded to two equivalent Cr(1), one Zn(1), and one Al(1) atom to form distorted SAlZnCr2 trigonal pyramids that share corners with six equivalent S(2)Al2ZnCr trigonal pyramids, corners with six equivalent S(1)AlZnCr2 trigonal pyramids,  an edgeedge with one S(1)AlZnCr2 trigonal pyramid, and edges with two equivalent S(2)Al2ZnCr trigonal pyramids. In the second S site, S(2) is bonded to one Cr(1), one Zn(1), and two equivalent Al(1) atoms to form distorted SAl2ZnCr trigonal pyramids that share corners with six equivalent S(2)Al2ZnCr trigonal pyramids, corners with six equivalent S(1)AlZnCr2 trigonal pyramids,  an edgeedge with one S(2)Al2ZnCr trigonal pyramid, and edges with two equivalent S(1)AlZnCr2 trigonal pyramids.