TlCrSe2 crystallizes in the trigonal R-3m space group. Cr(1) is bonded to six equivalent Se(1) atoms to form edge-sharing CrSe6 octahedra. Tl(1) is bonded in a linear geometry to two equivalent Se(1) atoms. Se(1) is bonded in a distorted rectangular see-saw-like geometry to three equivalent Cr(1) and one Tl(1) atom.
TlCrSe2 crystallizes in the trigonal R-3m space group. Cr(1) is bonded to six equivalent Se(1) atoms to form edge-sharing CrSe6 octahedra. All Cr(1)-Se(1) bond lengths are 2.51 Å. Tl(1) is bonded in a linear geometry to two equivalent Se(1) atoms. Both Tl(1)-Se(1) bond lengths are 3.19 Å. Se(1) is bonded in a distorted rectangular see-saw-like geometry to three equivalent Cr(1) and one Tl(1) atom.