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Tl3Ge crystallizes in the hexagonal P6_3/mmc space group. The structure is three-dimensional. Tl is bonded in a 2-coordinate geometry to six equivalent Tl and two equivalent Ge atoms. There are two shorter (3.39 Å) and four longer (3.41 Å) Tl–Tl bond lengths. Both Tl–Ge bond lengths are 3.32 Å. Ge is bonded in a 6-coordinate geometry to six equivalent Tl atoms.
Tl3Ge is alpha bismuth trifluoride structured and crystallizes in the tetragonal I4/mmm space group. The structure is three-dimensional. there are two inequivalent Tl sites. In the first Tl site, Tl is bonded in a distorted body-centered cubic geometry to four equivalent Tl and four equivalent Ge atoms. All Tl–Tl bond lengths are 3.32 Å. All Tl–Ge bond lengths are 3.32 Å. In the second Tl site, Tl is bonded in a body-centered cubic geometry to eight equivalent Tl atoms. Ge is bonded in a body-centered cubic geometry to eight equivalent Tl atoms.
Tl3Ge is Uranium Silicide structured and crystallizes in the cubic Pm-3m space group. The structure is three-dimensional. Tl is bonded to eight equivalent Tl and four equivalent Ge atoms to form distorted TlTl8Ge4 cuboctahedra that share corners with twelve equivalent TlTl8Ge4 cuboctahedra, edges with eight equivalent GeTl12 cuboctahedra, edges with sixteen equivalent TlTl8Ge4 cuboctahedra, faces with four equivalent GeTl12 cuboctahedra, and faces with fourteen equivalent TlTl8Ge4 cuboctahedra. All Tl–Tl bond lengths are 3.41 Å. All Tl–Ge bond lengths are 3.41 Å. Ge is bonded to twelve equivalent Tl atoms to form distorted GeTl12 cuboctahedra that share corners with twelve equivalent GeTl12 cuboctahedra, edges with twenty-four equivalent TlTl8Ge4 cuboctahedra, faces with six equivalent GeTl12 cuboctahedra, and faces with twelve equivalent TlTl8Ge4 cuboctahedra.