MgTiAlS4 is Spinel-derived structured and crystallizes in the orthorhombic Imma space group. Mg(1) is bonded to two equivalent S(1) and two equivalent S(2) atoms to form MgS4 tetrahedra that share corners with six equivalent Ti(1)S6 octahedra and corners with six equivalent Al(1)S6 octahedra. The corner-sharing octahedral tilt angles range from 56-59°. Ti(1) is bonded to two equivalent S(2) and four equivalent S(1) atoms to form TiS6 octahedra that share corners with six equivalent Mg(1)S4 tetrahedra, edges with two equivalent Ti(1)S6 octahedra, and edges with four equivalent Al(1)S6 octahedra. 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 Mg(1)S4 tetrahedra, edges with two equivalent Al(1)S6 octahedra, and edges with four equivalent Ti(1)S6 octahedra. There are two inequivalent S sites. In the first S site, S(1) is bonded to one Mg(1), two equivalent Ti(1), and one Al(1) atom to form distorted SMgTi2Al trigonal pyramids that share corners with six equivalent S(1)MgTi2Al trigonal pyramids, corners with six equivalent S(2)MgTiAl2 trigonal pyramids,  an edgeedge with one S(1)MgTi2Al trigonal pyramid, and edges with two equivalent S(2)MgTiAl2 trigonal pyramids. In the second S site, S(2) is bonded to one Mg(1), one Ti(1), and two equivalent Al(1) atoms to form distorted SMgTiAl2 trigonal pyramids that share corners with six equivalent S(1)MgTi2Al trigonal pyramids, corners with six equivalent S(2)MgTiAl2 trigonal pyramids,  an edgeedge with one S(2)MgTiAl2 trigonal pyramid, and edges with two equivalent S(1)MgTi2Al trigonal pyramids.
MgTiAlS4 is Spinel-derived structured and crystallizes in the orthorhombic Imma space group. Mg(1) is bonded to two equivalent S(1) and two equivalent S(2) atoms to form MgS4 tetrahedra that share corners with six equivalent Ti(1)S6 octahedra and corners with six equivalent Al(1)S6 octahedra. The corner-sharing octahedral tilt angles range from 56-59°. Both Mg(1)-S(1) bond lengths are 2.44 Å. Both Mg(1)-S(2) bond lengths are 2.43 Å. Ti(1) is bonded to two equivalent S(2) and four equivalent S(1) atoms to form TiS6 octahedra that share corners with six equivalent Mg(1)S4 tetrahedra, edges with two equivalent Ti(1)S6 octahedra, and edges with four equivalent Al(1)S6 octahedra. Both Ti(1)-S(2) bond lengths are 2.49 Å. All Ti(1)-S(1) bond lengths are 2.49 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 Mg(1)S4 tetrahedra, edges with two equivalent Al(1)S6 octahedra, and edges with four equivalent Ti(1)S6 octahedra. Both Al(1)-S(1) bond lengths are 2.45 Å. All Al(1)-S(2) bond lengths are 2.45 Å. There are two inequivalent S sites. In the first S site, S(1) is bonded to one Mg(1), two equivalent Ti(1), and one Al(1) atom to form distorted SMgTi2Al trigonal pyramids that share corners with six equivalent S(1)MgTi2Al trigonal pyramids, corners with six equivalent S(2)MgTiAl2 trigonal pyramids,  an edgeedge with one S(1)MgTi2Al trigonal pyramid, and edges with two equivalent S(2)MgTiAl2 trigonal pyramids. In the second S site, S(2) is bonded to one Mg(1), one Ti(1), and two equivalent Al(1) atoms to form distorted SMgTiAl2 trigonal pyramids that share corners with six equivalent S(1)MgTi2Al trigonal pyramids, corners with six equivalent S(2)MgTiAl2 trigonal pyramids,  an edgeedge with one S(2)MgTiAl2 trigonal pyramid, and edges with two equivalent S(1)MgTi2Al trigonal pyramids.