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Cr3Os crystallizes in the cubic Pm-3n space group. The structure is three-dimensional. Cr is bonded in a 6-coordinate geometry to two equivalent Cr and four equivalent Os atoms. Both Cr–Cr bond lengths are 2.32 Å. All Cr–Os bond lengths are 2.60 Å. Os is bonded to twelve equivalent Cr atoms to form a mixture of edge and face-sharing OsCr12 cuboctahedra.
Cr3Os crystallizes in the orthorhombic Cmmm space group. The structure is three-dimensional. there are two inequivalent Cr sites. In the first Cr site, Cr is bonded in a 8-coordinate geometry to two equivalent Cr and two equivalent Os atoms. Both Cr–Cr bond lengths are 2.40 Å. Both Cr–Os bond lengths are 2.58 Å. In the second Cr site, Cr is bonded in a distorted body-centered cubic geometry to eight Cr atoms. All Cr–Cr bond lengths are 2.58 Å. Os is bonded in a 4-coordinate geometry to four equivalent Cr atoms.