MgHo2S4 is Spinel-like structured and crystallizes in the orthorhombic Pnma space group. Mg(1) is bonded to one S(2), one S(3), and two equivalent S(1) atoms to form MgS4 tetrahedra that share corners with two equivalent Ho(1)S6 octahedra, corners with four equivalent Ho(2)S6 octahedra,  an edgeedge with one Ho(2)S6 octahedra, and edges with two equivalent Ho(1)S6 octahedra. The corner-sharing octahedral tilt angles range from 58-67°. There are two inequivalent Ho sites. In the first Ho site, Ho(1) is bonded to two equivalent S(1), two equivalent S(2), and two equivalent S(3) atoms to form HoS6 octahedra that share corners with four equivalent Ho(2)S6 octahedra, corners with two equivalent Mg(1)S4 tetrahedra, edges with two equivalent Ho(1)S6 octahedra, edges with two equivalent Ho(2)S6 octahedra, and edges with two equivalent Mg(1)S4 tetrahedra. The corner-sharing octahedral tilt angles range from 50-56°. In the second Ho site, Ho(2) is bonded to one S(2), one S(3), and four equivalent S(1) atoms to form HoS6 octahedra that share corners with four equivalent Ho(1)S6 octahedra, corners with four equivalent Ho(2)S6 octahedra, corners with four equivalent Mg(1)S4 tetrahedra, edges with two equivalent Ho(1)S6 octahedra, and  an edgeedge with one Mg(1)S4 tetrahedra. The corner-sharing octahedral tilt angles range from 45-56°. There are three inequivalent S sites. In the first S site, S(1) is bonded in a rectangular see-saw-like geometry to one Mg(1), one Ho(1), and two equivalent Ho(2) atoms. In the second S site, S(2) is bonded in a rectangular see-saw-like geometry to one Mg(1), one Ho(2), and two equivalent Ho(1) atoms. In the third S site, S(3) is bonded to one Mg(1), one Ho(2), and two equivalent Ho(1) atoms to form distorted corner-sharing SHo3Mg tetrahedra.
MgHo2S4 is Spinel-like structured and crystallizes in the orthorhombic Pnma space group. Mg(1) is bonded to one S(2), one S(3), and two equivalent S(1) atoms to form MgS4 tetrahedra that share corners with two equivalent Ho(1)S6 octahedra, corners with four equivalent Ho(2)S6 octahedra,  an edgeedge with one Ho(2)S6 octahedra, and edges with two equivalent Ho(1)S6 octahedra. The corner-sharing octahedral tilt angles range from 58-67°. The Mg(1)-S(2) bond length is 2.47 Å. The Mg(1)-S(3) bond length is 2.38 Å. Both Mg(1)-S(1) bond lengths are 2.45 Å. There are two inequivalent Ho sites. In the first Ho site, Ho(1) is bonded to two equivalent S(1), two equivalent S(2), and two equivalent S(3) atoms to form HoS6 octahedra that share corners with four equivalent Ho(2)S6 octahedra, corners with two equivalent Mg(1)S4 tetrahedra, edges with two equivalent Ho(1)S6 octahedra, edges with two equivalent Ho(2)S6 octahedra, and edges with two equivalent Mg(1)S4 tetrahedra. The corner-sharing octahedral tilt angles range from 50-56°. Both Ho(1)-S(1) bond lengths are 2.74 Å. Both Ho(1)-S(2) bond lengths are 2.73 Å. Both Ho(1)-S(3) bond lengths are 2.68 Å. In the second Ho site, Ho(2) is bonded to one S(2), one S(3), and four equivalent S(1) atoms to form HoS6 octahedra that share corners with four equivalent Ho(1)S6 octahedra, corners with four equivalent Ho(2)S6 octahedra, corners with four equivalent Mg(1)S4 tetrahedra, edges with two equivalent Ho(1)S6 octahedra, and  an edgeedge with one Mg(1)S4 tetrahedra. The corner-sharing octahedral tilt angles range from 45-56°. The Ho(2)-S(2) bond length is 2.71 Å. The Ho(2)-S(3) bond length is 2.73 Å. There are two shorter (2.74 Å) and two longer (2.79 Å) Ho(2)-S(1) bond lengths. There are three inequivalent S sites. In the first S site, S(1) is bonded in a rectangular see-saw-like geometry to one Mg(1), one Ho(1), and two equivalent Ho(2) atoms. In the second S site, S(2) is bonded in a rectangular see-saw-like geometry to one Mg(1), one Ho(2), and two equivalent Ho(1) atoms. In the third S site, S(3) is bonded to one Mg(1), one Ho(2), and two equivalent Ho(1) atoms to form distorted corner-sharing SHo3Mg tetrahedra.