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Nb2CrOs crystallizes in the orthorhombic Immm space group. The structure is one-dimensional and consists of two Nb2CrOs ribbons oriented in the (1, 0, 0) direction. Nb is bonded in a linear geometry to one Cr and one Os atom. The Nb–Cr bond length is 2.74 Å. The Nb–Os bond length is 2.30 Å. Cr is bonded in a linear geometry to two equivalent Nb atoms. Os is bonded in a linear geometry to two equivalent Nb atoms.
Nb2CrOs is Heusler structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Nb is bonded in a distorted body-centered cubic geometry to four equivalent Cr and four equivalent Os atoms. All Nb–Cr bond lengths are 2.73 Å. All Nb–Os bond lengths are 2.73 Å. Cr is bonded in a 8-coordinate geometry to eight equivalent Nb and six equivalent Os atoms. All Cr–Os bond lengths are 3.15 Å. Os is bonded in a distorted body-centered cubic geometry to eight equivalent Nb and six equivalent Cr atoms.