Nanostructures down to a few ten nanometers in size have been fabricated with Langmuir-Blodgett (LB) films and self-assembled monolayers (SAMs) using scanning probe microscope lithography. The SAMs have been prepared with organosilane and bipolar amphiphiles, alkanethiol molecules as ultrathin resists on Si and ALI substrates. The LB films on silicon substrates using both the polymer of thiophene derivatives and the mixture of palmitic acid and hexadecylamine were prepared and fabricated. The effect of functional groups of molecules on the atomic force microscope (AFM) anodization has been studied in the optimized process conditions. Applied voltage between the AFM tip and sample, the scanning speed and the relative humidity in the laboratory are also important factors for nano meter-scale lithography of the ultrathin films. The STM lithography with an octadecanethiol SAM on Au film in the air was carried out at the pulse mode of tip bias with respect to the suitability of STM lithography. The high structural orderness and perfect thickness of ultrathin organic molecular assemblies are the major advantages as required for nanoscale lithography. (C) 2002 Elsevier Science B.V. All rights reserved.