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Sm2C is trigonal omega-like structured and crystallizes in the trigonal R-3m space group. The structure is two-dimensional and consists of three Sm2C sheets oriented in the (0, 0, 1) direction. Sm2+ is bonded in a distorted T-shaped geometry to three equivalent C4- atoms. All Sm–C bond lengths are 2.53 Å. C4- is bonded to six equivalent Sm2+ atoms to form edge-sharing CSm6 octahedra.
Sm2C(NO)2 crystallizes in the trigonal P-3m1 space group. The structure is three-dimensional. Sm3+ is bonded in a 7-coordinate geometry to three equivalent N3- and four equivalent O2- atoms. All Sm–N bond lengths are 2.65 Å. There are three shorter (2.31 Å) and one longer (2.35 Å) Sm–O bond lengths. C4+ is bonded in a linear geometry to two equivalent N3- atoms. Both C–N bond lengths are 1.24 Å. N3- is bonded in a 1-coordinate geometry to three equivalent Sm3+ and one C4+ atom. O2- is bonded to four equivalent Sm3+ atoms to form a mixture of corner and edge-sharing OSm4 tetrahedra.