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TlCrTe2 crystallizes in the trigonal P-3m1 space group. The structure is three-dimensional. Cr3+ is bonded to six equivalent Te2- atoms to form edge-sharing CrTe6 octahedra. All Cr–Te bond lengths are 2.78 Å. Tl1+ is bonded in a 6-coordinate geometry to six equivalent Te2- atoms. All Tl–Te bond lengths are 3.49 Å. Te2- is bonded in a 6-coordinate geometry to three equivalent Cr3+ and three equivalent Tl1+ atoms.
TlCr5Te8 is Orthorhombic Perovskite-like structured and crystallizes in the monoclinic Cm space group. The structure is three-dimensional. there are five inequivalent Cr3+ sites. In the first Cr3+ site, Cr3+ is bonded to six Te2- atoms to form a mixture of corner, edge, and face-sharing CrTe6 octahedra. The corner-sharing octahedra tilt angles range from 50–51°. There are a spread of Cr–Te bond distances ranging from 2.69–2.80 Å. In the second Cr3+ site, Cr3+ is bonded to six Te2- atoms to form a mixture of corner, edge, and face-sharing CrTe6 octahedra. The corner-sharing octahedra tilt angles range from 50–51°. There are a spread of Cr–Te bond distances ranging from 2.70–2.81 Å. In the third Cr3+ site, Cr3+ is bonded to six Te2- atoms to form a mixture of corner, edge, and face-sharing CrTe6 octahedra. The corner-sharing octahedra tilt angles range from 50–51°. There are a spread of Cr–Te bond distances ranging from 2.71–2.86 Å. In the fourth Cr3+ site, Cr3+ is bonded to six Te2- atoms to form a mixture of corner, edge, and face-sharing CrTe6 octahedra. The corner-sharing octahedra tilt angles range from 50–51°. There are a spread of Cr–Te bond distances ranging from 2.71–2.86 Å. In the fifth Cr3+ site, Cr3+ is bonded to six Te2- atoms to form a mixture of corner and edge-sharing CrTe6 octahedra. The corner-sharing octahedral tilt angles are 50°. There are two shorter (2.72 Å) and four longer (2.74 Å) Cr–Te bond lengths. Tl1+ is bonded in a 12-coordinate geometry to ten Te2- atoms. There are a spread of Tl–Te bond distances ranging from 3.62–4.33 Å. There are eight inequivalent Te2- sites. In the first Te2- site, Te2- is bonded in a 3-coordinate geometry to three Cr3+ and two equivalent Tl1+ atoms. In the second Te2- site, Te2- is bonded in a 5-coordinate geometry to three Cr3+ and two equivalent Tl1+ atoms. In the third Te2- site, Te2- is bonded in a 3-coordinate geometry to three Cr3+ and two equivalent Tl1+ atoms. In the fourth Te2- site, Te2- is bonded in a 3-coordinate geometry to three Cr3+ and two equivalent Tl1+ atoms. In the fifth Te2- site, Te2- is bonded in a 5-coordinate geometry to five Cr3+ atoms. In the sixth Te2- site, Te2- is bonded in a 5-coordinate geometry to five Cr3+ atoms. In the seventh Te2- site, Te2- is bonded in a 4-coordinate geometry to four Cr3+ and one Tl1+ atom. In the eighth Te2- site, Te2- is bonded in a distorted rectangular see-saw-like geometry to four Cr3+ and one Tl1+ atom.