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Li2CaAl crystallizes in the orthorhombic Immm space group. The structure is one-dimensional and consists of two Li2CaAl ribbons oriented in the (0, 1, 0) direction. Li is bonded in a distorted linear geometry to one Ca and one Al atom. The Li–Ca bond length is 3.43 Å. The Li–Al bond length is 2.78 Å. Ca is bonded in a linear geometry to two equivalent Li atoms. Al is bonded in a linear geometry to two equivalent Li atoms.
Li2CaAl is Heusler structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Li is bonded in a body-centered cubic geometry to four equivalent Ca and four equivalent Al atoms. All Li–Ca bond lengths are 3.02 Å. All Li–Al bond lengths are 3.02 Å. Ca is bonded in a 8-coordinate geometry to eight equivalent Li and six equivalent Al atoms. All Ca–Al bond lengths are 3.49 Å. Al is bonded in a distorted body-centered cubic geometry to eight equivalent Li and six equivalent Ca atoms.