In this research, (3-alkyl benzimidazalium)-TCNQ complexes were synthesized to obtain the necessary components for Langmuir-Blodgett Technique. (3-Alkyl benzimidazolium)-TCNQ complexes were prepared by the reaction of LiTCNQ with 3-alkyl benzimidazolium bromides and the products were confirmed by elemental analysis. FT-IR, UV-Visible spectroscopies FT-IR spectra of (3-alkyl benzimidazolium)-TCNQ(1 : 2) complexes were characterized by a broad band with a maximum at about 2900cm^-1 appears and were ascribed to electronic rather than vibrational absorption.