Octadecyltrimethylammonium-TCNQ(1:1) complex was synthesized by the reaction of LiTCNQ with octadecyltrimethylammonium bromide and the reaction product was identified with FT-IR and UV/Vis spectroscopies. In order to prepare the LB films, π-A isotherm characteristics of octadecyltrimethylammonium-TCNQ(1:1) complex were investigated. The LB films of octadecyltrimethylammonium-TCNQ(1:1) complex were formed on various substrates and the formation of ultrathin films of octadecyltrimethylammonium-TCNQ(1:1) complex was confirmed by using FT-IR and UV-Vis spectroscopies.