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TmGe crystallizes in the orthorhombic Cmcm space group. The structure is three-dimensional. Tm is bonded in a 5-coordinate geometry to seven equivalent Ge atoms. There are a spread of Tm–Ge bond distances ranging from 2.91–3.19 Å. Ge is bonded in a 5-coordinate geometry to seven equivalent Tm and two equivalent Ge atoms. Both Ge–Ge bond lengths are 2.69 Å.
LiTm4Ge4 is delta Molybdenum Boride-derived structured and crystallizes in the orthorhombic Pnma space group. The structure is three-dimensional. Li is bonded in a 3-coordinate geometry to five Ge atoms. There are a spread of Li–Ge bond distances ranging from 2.66–3.11 Å. There are two inequivalent Tm sites. In the first Tm site, Tm is bonded in a 6-coordinate geometry to six Ge atoms. There are a spread of Tm–Ge bond distances ranging from 2.81–2.99 Å. In the second Tm site, Tm is bonded in a 7-coordinate geometry to seven Ge atoms. There are a spread of Tm–Ge bond distances ranging from 2.93–3.33 Å. There are three inequivalent Ge sites. In the first Ge site, Ge is bonded in a 1-coordinate geometry to one Li, six Tm, and one Ge atom. The Ge–Ge bond length is 2.55 Å. In the second Ge site, Ge is bonded in a 9-coordinate geometry to two equivalent Li, six Tm, and one Ge atom. In the third Ge site, Ge is bonded in a 9-coordinate geometry to one Li, seven Tm, and one Ge atom. The Ge–Ge bond length is 2.65 Å.