Cr4Te3Se is Caswellsilverite-like structured and crystallizes in the hexagonal P-6m2 space group. There are two inequivalent Cr sites. In the first Cr site, Cr(1) is bonded to three equivalent Te(2) and three equivalent Se(1) atoms to form CrTe3Se3 octahedra that share corners with six equivalent Cr(1)Te3Se3 octahedra, corners with six equivalent Cr(2)Te6 octahedra, edges with six equivalent Cr(1)Te3Se3 octahedra,  a faceface with one Cr(1)Te3Se3 octahedra, and  a faceface with one Cr(2)Te6 octahedra. The corner-sharing octahedral tilt angles range from 49-50°. In the second Cr site, Cr(2) is bonded to three equivalent Te(1) and three equivalent Te(2) atoms to form CrTe6 octahedra that share corners with six equivalent Cr(1)Te3Se3 octahedra, corners with six equivalent Cr(2)Te6 octahedra, edges with six equivalent Cr(2)Te6 octahedra,  a faceface with one Cr(1)Te3Se3 octahedra, and  a faceface with one Cr(2)Te6 octahedra. The corner-sharing octahedral tilt angles are 49°. There are two inequivalent Te sites. In the first Te site, Te(1) is bonded in a 6-coordinate geometry to six equivalent Cr(2) atoms. In the second Te site, Te(2) is bonded in a 6-coordinate geometry to three equivalent Cr(1) and three equivalent Cr(2) atoms. Se(1) is bonded in a 6-coordinate geometry to six equivalent Cr(1) atoms.
Cr4Te3Se is Caswellsilverite-like structured and crystallizes in the hexagonal P-6m2 space group. There are two inequivalent Cr sites. In the first Cr site, Cr(1) is bonded to three equivalent Te(2) and three equivalent Se(1) atoms to form CrTe3Se3 octahedra that share corners with six equivalent Cr(1)Te3Se3 octahedra, corners with six equivalent Cr(2)Te6 octahedra, edges with six equivalent Cr(1)Te3Se3 octahedra,  a faceface with one Cr(1)Te3Se3 octahedra, and  a faceface with one Cr(2)Te6 octahedra. The corner-sharing octahedral tilt angles range from 49-50°. All Cr(1)-Te(2) bond lengths are 2.84 Å. All Cr(1)-Se(1) bond lengths are 2.77 Å. In the second Cr site, Cr(2) is bonded to three equivalent Te(1) and three equivalent Te(2) atoms to form CrTe6 octahedra that share corners with six equivalent Cr(1)Te3Se3 octahedra, corners with six equivalent Cr(2)Te6 octahedra, edges with six equivalent Cr(2)Te6 octahedra,  a faceface with one Cr(1)Te3Se3 octahedra, and  a faceface with one Cr(2)Te6 octahedra. The corner-sharing octahedral tilt angles are 49°. All Cr(2)-Te(1) bond lengths are 2.82 Å. All Cr(2)-Te(2) bond lengths are 2.83 Å. There are two inequivalent Te sites. In the first Te site, Te(1) is bonded in a 6-coordinate geometry to six equivalent Cr(2) atoms. In the second Te site, Te(2) is bonded in a 6-coordinate geometry to three equivalent Cr(1) and three equivalent Cr(2) atoms. Se(1) is bonded in a 6-coordinate geometry to six equivalent Cr(1) atoms.