CsMo3I7 crystallizes in the trigonal P-31c space group. There are two inequivalent Cs sites. In the first Cs site, Cs(1) is bonded in a 6-coordinate geometry to six equivalent I(2) atoms. In the second Cs site, Cs(2) is bonded to six equivalent I(2) and six equivalent I(3) atoms to form CsI12 cuboctahedra that share corners with six equivalent Mo(1)Mo4I5 square pyramids and faces with six equivalent Mo(1)Mo4I5 square pyramids. Mo(1) is bonded to four equivalent Mo(1), one I(1), one I(2), and three equivalent I(3) atoms to form distorted MoMo4I5 square pyramids that share  a cornercorner with one Cs(2)I12 cuboctahedra,  a faceface with one Cs(2)I12 cuboctahedra, and faces with five equivalent Mo(1)Mo4I5 square pyramids. There are three inequivalent I sites. In the first I site, I(3) is bonded in a 4-coordinate geometry to one Cs(2) and three equivalent Mo(1) atoms. In the second I site, I(1) is bonded in a 3-coordinate geometry to three equivalent Mo(1) atoms. In the third I site, I(2) is bonded in a 3-coordinate geometry to one Cs(1), one Cs(2), and one Mo(1) atom.
CsMo3I7 crystallizes in the trigonal P-31c space group. There are two inequivalent Cs sites. In the first Cs site, Cs(1) is bonded in a 6-coordinate geometry to six equivalent I(2) atoms. All Cs(1)-I(2) bond lengths are 3.97 Å. In the second Cs site, Cs(2) is bonded to six equivalent I(2) and six equivalent I(3) atoms to form CsI12 cuboctahedra that share corners with six equivalent Mo(1)Mo4I5 square pyramids and faces with six equivalent Mo(1)Mo4I5 square pyramids. All Cs(2)-I(2) bond lengths are 4.39 Å. All Cs(2)-I(3) bond lengths are 4.14 Å. Mo(1) is bonded to four equivalent Mo(1), one I(1), one I(2), and three equivalent I(3) atoms to form distorted MoMo4I5 square pyramids that share  a cornercorner with one Cs(2)I12 cuboctahedra,  a faceface with one Cs(2)I12 cuboctahedra, and faces with five equivalent Mo(1)Mo4I5 square pyramids. There is one shorter (2.68 Å) and three longer (2.71 Å) Mo(1)-Mo(1) bond lengths. The Mo(1)-I(1) bond length is 2.80 Å. The Mo(1)-I(2) bond length is 2.89 Å. There are a spread of Mo(1)-I(3) bond distances ranging from 2.79-2.82 Å. There are three inequivalent I sites. In the first I site, I(3) is bonded in a 4-coordinate geometry to one Cs(2) and three equivalent Mo(1) atoms. In the second I site, I(1) is bonded in a 3-coordinate geometry to three equivalent Mo(1) atoms. In the third I site, I(2) is bonded in a 3-coordinate geometry to one Cs(1), one Cs(2), and one Mo(1) atom.