Ultra-thin films of hexyltriphenylphosphonium-TCNQ(1:1) complex were formed on various substrates by Langmuir-Blodgett technique, where hexyltriphenylphosphonium-TCNQ(1:1) complex was synthesized by attaching hexyltriphenylphosphonium group to TCNQ. The reaction product was identified with FT-IR, and UV-Vis absorption spectroscopies. The formation of ultra-thin films of hexyltriphenylphosphonium-TCNQ(1:1) complex was confirmed also by FT-IR, and UV/Vis absorption spectroscopies.