New Schiff-base compounds N-(3,4-dimethoxybenzylidene)-4-methoxyaniline (1) and N-(3,4-dimethoxybenzylidene)-4-ethoxyaniline (2) were synthesized and characterized by elemental analyses (CHN) and FT-IR spectroscopic techniques. Crystal structures of 1 and 2 were obtained by single-crystal X-ray diffraction. Compound 1 crystallizes in the monoclinic, space group P2₁ with two independent molecules (A and B), with unit cell parameters: a = 14.8198(4), b = 7.1656(2), c = 13.2982(4) Ǻ, β = 103.289(2)°, V = 1374.36(7) Ǻ³ and Z = 4 and compound 2 crystallizes in the monoclinic space group P2₁/n with unit cell parameters: a = 16.5638(6), b = 7.3546(2), c = 12.7449(4) Ǻ, β = 106.021(4)°, V = 1492.28(9) Ǻ³ and Z = 4.