Two 1-methyl-1H-benzo[d]imidazole derivatives, C_（18）H_（14）CuN_4O_4·C_4H_8O_2（1） and C_9H_9N_3O（2）, have been synthesized and characterized by NMR, MS, FT-IR, elementary analysis and X-ray single-crystal diffraction. Compound 1 crystallizes in monoclinic, space group P2_1/n with a = 9.6888（3）, b = 7.3772（2）, c = 14.3277（4）A, β = 95.819（3）°, V = 1018.81（5） A3, M_r = 501.98, Z = 2, D_c = 1.636 g/cm^3, F（000） = 518, μ = 1.123 mm^（-1）, MoKα radiation（λ = 0.71073 A）, the final R = 0.0325 and wR = 0.0859 for 1821 observed reflections with I 〉 2σ（I）. Compound 2 crystallizes in monoclinic, space group C2/c with a = 14.2908（14）, b = 14.4268（13）, c = 8.4802（6） A, β = 108.513（9）o, V = 1657.9（3） A3, M_r = 175.19, Z = 8, D_c = 1.404 g/cm^3, F（000） = 736, μ = 0.097 mm^（-1）, Mo Kα radiation（λ = 0.71073 A）, the final R = 0.0563 and wR = 0.1531 for 1231 observed reflections with I 〉 2σ（I）. Intermolecular（N-H···N, N-H···O） and intramolecular（N-H···N, C-H···O） hydrogen bonds, as well as C-H···π and π-π stacking interactions, help to stabilize the crystal structure of compound 2.
