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Ca2HgTl crystallizes in the orthorhombic Immm space group. The structure is one-dimensional and consists of two Ca2HgTl ribbons oriented in the (1, 0, 0) direction. Ca is bonded in a linear geometry to one Hg and one Tl atom. The Ca–Hg bond length is 3.28 Å. The Ca–Tl bond length is 3.04 Å. Hg is bonded in a linear geometry to two equivalent Ca atoms. Tl is bonded in a linear geometry to two equivalent Ca atoms.
Ca2HgTl is Heusler structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Ca is bonded in a body-centered cubic geometry to four equivalent Hg and four equivalent Tl atoms. All Ca–Hg bond lengths are 3.33 Å. All Ca–Tl bond lengths are 3.33 Å. Hg is bonded in a body-centered cubic geometry to eight equivalent Ca atoms. Tl is bonded in a body-centered cubic geometry to eight equivalent Ca atoms.