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CaB6 is Calcium hexaboride structured and crystallizes in the cubic Pm-3m space group. The structure is three-dimensional. Ca is bonded in a 1-coordinate geometry to twenty-four equivalent B atoms. All Ca–B bond lengths are 3.05 Å. B is bonded in a 1-coordinate geometry to four equivalent Ca and five equivalent B atoms. There is one shorter (1.68 Å) and four longer (1.75 Å) B–B bond length.
CaB2 is hexagonal omega structure structured and crystallizes in the hexagonal P6/mmm space group. The structure is three-dimensional. Ca is bonded to twelve equivalent B atoms to form a mixture of edge and face-sharing CaB12 cuboctahedra. All Ca–B bond lengths are 2.76 Å. B is bonded in a 9-coordinate geometry to six equivalent Ca and three equivalent B atoms. All B–B bond lengths are 1.86 Å.