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Ca2N is trigonal omega-like structured and crystallizes in the trigonal R-3m space group. The structure is two-dimensional and consists of three Ca2N sheets oriented in the (0, 0, 1) direction. Ca is bonded in a distorted T-shaped geometry to three equivalent N atoms. All Ca–N bond lengths are 2.43 Å. N is bonded to six equivalent Ca atoms to form edge-sharing NCa6 octahedra.
Ca3N2 crystallizes in the hexagonal P6_3/mmc space group. The structure is two-dimensional and consists of two Ca2N sheets oriented in the (0, 0, 1) direction and two CaN sheets oriented in the (0, 0, 1) direction. In each Ca2N sheet, Ca2+ is bonded in a 3-coordinate geometry to three equivalent N3- atoms. All Ca–N bond lengths are 2.52 Å. N3- is bonded to six equivalent Ca2+ atoms to form distorted edge-sharing NCa6 octahedra. In each CaN sheet, Ca2+ is bonded in a trigonal planar geometry to three equivalent N3- atoms. All Ca–N bond lengths are 2.25 Å. N3- is bonded in a trigonal planar geometry to three equivalent Ca2+ atoms.