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HfZrOs2 crystallizes in the orthorhombic Immm space group. The structure is one-dimensional and consists of two HfZrOs2 ribbons oriented in the (1, 0, 0) direction. Hf is bonded in a linear geometry to two equivalent Os atoms. Both Hf–Os bond lengths are 2.42 Å. Zr is bonded in a linear geometry to two equivalent Os atoms. Both Zr–Os bond lengths are 2.41 Å. Os is bonded in a linear geometry to one Hf and one Zr atom.
HfZrOs2 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 eight equivalent Os atoms. All Hf–Os bond lengths are 2.84 Å. Zr is bonded in a body-centered cubic geometry to eight equivalent Os atoms. All Zr–Os bond lengths are 2.84 Å. Os is bonded in a body-centered cubic geometry to four equivalent Hf and four equivalent Zr atoms.