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MgCN2 crystallizes in the tetragonal I-42d space group. The structure is three-dimensional. Mg2+ is bonded in a 4-coordinate geometry to four equivalent N3- atoms. All Mg–N bond lengths are 2.09 Å. C4+ is bonded to four equivalent N3- atoms to form corner-sharing CN4 tetrahedra. All C–N bond lengths are 1.51 Å. N3- is bonded in a 4-coordinate geometry to two equivalent Mg2+ and two equivalent C4+ atoms.
MgCN2 crystallizes in the trigonal R-3m space group. The structure is three-dimensional. Mg2+ is bonded to six equivalent N3- atoms to form edge-sharing MgN6 octahedra. All Mg–N bond lengths are 2.22 Å. C4+ is bonded in a linear geometry to two equivalent N3- atoms. Both C–N bond lengths are 1.23 Å. N3- is bonded to three equivalent Mg2+ and one C4+ atom to form a mixture of distorted edge and corner-sharing NMg3C trigonal pyramids.