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Mn2CrSi crystallizes in the orthorhombic Immm space group. The structure is one-dimensional and consists of two Mn2CrSi ribbons oriented in the (0, 1, 0) direction. Cr is bonded in a linear geometry to two equivalent Mn atoms. Both Cr–Mn bond lengths are 2.77 Å. Mn is bonded in a linear geometry to one Cr and one Si atom. The Mn–Si bond length is 2.32 Å. Si is bonded in a linear geometry to two equivalent Mn atoms.
Mn2CrSi is Heusler structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Cr is bonded in a distorted body-centered cubic geometry to eight equivalent Mn atoms. All Cr–Mn bond lengths are 2.42 Å. Mn is bonded in a body-centered cubic geometry to four equivalent Cr and four equivalent Si atoms. All Mn–Si bond lengths are 2.42 Å. Si is bonded in a body-centered cubic geometry to eight equivalent Mn atoms.