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CaYZn2 crystallizes in the orthorhombic Immm space group. The structure is one-dimensional and consists of two CaYZn2 ribbons oriented in the (1, 0, 0) direction. Ca is bonded in a linear geometry to two equivalent Zn atoms. Both Ca–Zn bond lengths are 3.16 Å. Y is bonded in a linear geometry to two equivalent Zn atoms. Both Y–Zn bond lengths are 3.02 Å. Zn is bonded in a linear geometry to one Ca and one Y atom.
CaYZn2 is Heusler structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Ca is bonded in a body-centered cubic geometry to eight equivalent Zn atoms. All Ca–Zn bond lengths are 3.14 Å. Y is bonded in a body-centered cubic geometry to eight equivalent Zn atoms. All Y–Zn bond lengths are 3.14 Å. Zn is bonded in a body-centered cubic geometry to four equivalent Ca and four equivalent Y atoms.