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LiCrRh2 crystallizes in the orthorhombic Immm space group. The structure is one-dimensional and consists of two LiCrRh2 ribbons oriented in the (0, 1, 0) direction. Li is bonded in a linear geometry to two equivalent Rh atoms. Both Li–Rh bond lengths are 2.67 Å. Cr is bonded in a linear geometry to two equivalent Rh atoms. Both Cr–Rh bond lengths are 2.04 Å. Rh is bonded in a linear geometry to one Li and one Cr atom.
LiCrRh2 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 eight equivalent Rh atoms. All Li–Rh bond lengths are 2.55 Å. Cr is bonded in a distorted body-centered cubic geometry to eight equivalent Rh atoms. All Cr–Rh bond lengths are 2.55 Å. Rh is bonded in a body-centered cubic geometry to four equivalent Li and four equivalent Cr atoms.