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SiC2N4 crystallizes in the cubic Pn-3m space group. The structure is three-dimensional. Si4+ is bonded in a tetrahedral geometry to four equivalent N3- atoms. All Si–N bond lengths are 1.69 Å. C4+ is bonded in a linear geometry to two equivalent N3- atoms. Both C–N bond lengths are 1.21 Å. N3- is bonded in a linear geometry to one Si4+ and one C4+ atom.
KLaSi(CN2)4 crystallizes in the orthorhombic P2_12_12 space group. The structure is three-dimensional. K1+ is bonded in a 6-coordinate geometry to six N3- atoms. There are a spread of K–N bond distances ranging from 2.94–3.14 Å. La3+ is bonded in a 8-coordinate geometry to eight N3- atoms. There are a spread of La–N bond distances ranging from 2.54–2.76 Å. Si4+ is bonded in a tetrahedral geometry to four N3- atoms. There is two shorter (1.72 Å) and two longer (1.73 Å) Si–N bond length. There are two inequivalent C4+ sites. In the first C4+ site, C4+ is bonded in a linear geometry to two N3- atoms. There is one shorter (1.20 Å) and one longer (1.27 Å) C–N bond length. In the second C4+ site, C4+ is bonded in a linear geometry to two N3- atoms. There is one shorter (1.20 Å) and one longer (1.27 Å) C–N bond length. There are four inequivalent N3- sites. In the first N3- site, N3- is bonded in a distorted bent 120 degrees geometry to one K1+, one La3+, one Si4+, and one C4+ atom. In the second N3- site, N3- is bonded in a 3-coordinate geometry to one K1+, one La3+, and one C4+ atom. In the third N3- site, N3- is bonded in a 3-coordinate geometry to one K1+, one La3+, and one C4+ atom. In the fourth N3- site, N3- is bonded in a 2-coordinate geometry to one La3+, one Si4+, and one C4+ atom.