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Hf2FeRh crystallizes in the orthorhombic Immm space group. The structure is one-dimensional and consists of two Hf2FeRh ribbons oriented in the (1, 0, 0) direction. Hf is bonded in a linear geometry to one Fe and one Rh atom. The Hf–Fe bond length is 2.11 Å. The Hf–Rh bond length is 2.32 Å. Fe is bonded in a linear geometry to two equivalent Hf atoms. Rh is bonded in a linear geometry to two equivalent Hf atoms.
Hf2FeRh is Heusler structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Hf is bonded in a body-centered cubic geometry to four equivalent Fe and four equivalent Rh atoms. All Hf–Fe bond lengths are 2.79 Å. All Hf–Rh bond lengths are 2.79 Å. Fe is bonded in a distorted body-centered cubic geometry to eight equivalent Hf atoms. Rh is bonded in a body-centered cubic geometry to eight equivalent Hf atoms.