SMI2(THF)2 reacts with potassium carbazole (KC12H8N, KCbz) in a 1:2 ratio at room temperature in THF to form (C12H8N)2SM(THF)4, 1.1 reacts with N-methylimidazole (N-MeIm) in a 1:4 ratio at room temperature in THF to form (C12H8N)2SM(N-MeIM)4, 2. X-ray crystallographic studies on 1 and 2 show that both have distorted octahedral structures but that (Cbz)2SM(THF)4 crystallizes as the cis isomer (N-Sm-N: 109.8(1)-degrees) and (Cbz)2SM(N-Melm)4 crystallizes as the trans isomer (N(Cbz)-Sm-N(Cbz)): 151.7(3) and 159.2(5)-degrees). 1 crystallizes from hot THF in space group P1BAR [C(1/i); No. 2] with unit cell parameters at 173 K of a = 9.8862(9) angstrom, b = 10.3285(7) angstrom, c = 18.3670(16) angstrom, alpha = 100.368(6)-degrees, beta = 98.522(7)-degrees, gamma = 102.898(6)-degrees, V = 1763.2(3) angstrom3, and Z = 2 with D(calcd) = 1.45 g cm-3. Least-squares refinement of the model based on 7577 observed reflections (\F(o)\ > 3.0sigma(\F(o)\)) converged to a final R(F) = 3.0%. 2 crystallized from THF/benzene in space group P3BAR with unit cell parameters at 163 K of a = 26.759(2) angstrom, c = 27.796(4) angstrom, V = 17 236(3) angstrom3, and Z = 18 with D(calcd) = 1.443 g CM-3. Least-squares refinement of the model based on 5505 observed reflections (\F(o)\ > 3.0sigma([F(o)\)) converged to a final R(F) = 6.5 %. The average Sm-N(Cbz) distances in 1 and 2 are 2.565(13) and 2.591(3) angstrom, respectively. The average Sm-O(THF) distance in 1 is 2.582(7) angstrom; the average Sm-N(N-MeIm) distance in 2 is 2.685(14) angstrom.