MgTiS2 is Caswellsilverite-like structured and crystallizes in the monoclinic Cm space group. Mg(1) is bonded to three equivalent S(1) and three equivalent S(2) atoms to form distorted MgS6 pentagonal pyramids that share corners with nine equivalent Ti(1)S6 octahedra, edges with three equivalent Ti(1)S6 octahedra, edges with six equivalent Mg(1)S6 pentagonal pyramids, and  a faceface with one Ti(1)S6 octahedra. The corner-sharing octahedral tilt angles range from 2-46°. Ti(1) is bonded to three equivalent S(1) and three equivalent S(2) atoms to form TiS6 octahedra that share corners with nine equivalent Mg(1)S6 pentagonal pyramids, edges with six equivalent Ti(1)S6 octahedra, edges with three equivalent Mg(1)S6 pentagonal pyramids, and  a faceface with one Mg(1)S6 pentagonal pyramid. There are two inequivalent S sites. In the first S site, S(1) is bonded to three equivalent Mg(1) and three equivalent Ti(1) atoms to form a mixture of edge, corner, and face-sharing SMg3Ti3 octahedra. In the second S site, S(2) is bonded to three equivalent Mg(1) and three equivalent Ti(1) atoms to form a mixture of distorted edge, corner, and face-sharing SMg3Ti3 pentagonal pyramids. The corner-sharing octahedral tilt angles range from 0-45°.
MgTiS2 is Caswellsilverite-like structured and crystallizes in the monoclinic Cm space group. Mg(1) is bonded to three equivalent S(1) and three equivalent S(2) atoms to form distorted MgS6 pentagonal pyramids that share corners with nine equivalent Ti(1)S6 octahedra, edges with three equivalent Ti(1)S6 octahedra, edges with six equivalent Mg(1)S6 pentagonal pyramids, and  a faceface with one Ti(1)S6 octahedra. The corner-sharing octahedral tilt angles range from 2-46°. There are two shorter (2.60 Å) and one longer (2.65 Å) Mg(1)-S(1) bond length. There is one shorter (2.61 Å) and two longer (2.63 Å) Mg(1)-S(2) bond lengths. Ti(1) is bonded to three equivalent S(1) and three equivalent S(2) atoms to form TiS6 octahedra that share corners with nine equivalent Mg(1)S6 pentagonal pyramids, edges with six equivalent Ti(1)S6 octahedra, edges with three equivalent Mg(1)S6 pentagonal pyramids, and  a faceface with one Mg(1)S6 pentagonal pyramid. All Ti(1)-S(1) bond lengths are 2.52 Å. All Ti(1)-S(2) bond lengths are 2.51 Å. There are two inequivalent S sites. In the first S site, S(1) is bonded to three equivalent Mg(1) and three equivalent Ti(1) atoms to form a mixture of edge, corner, and face-sharing SMg3Ti3 octahedra. In the second S site, S(2) is bonded to three equivalent Mg(1) and three equivalent Ti(1) atoms to form a mixture of distorted edge, corner, and face-sharing SMg3Ti3 pentagonal pyramids. The corner-sharing octahedral tilt angles range from 0-45°.