Organic thin-film transistors are attracting a great deal of attention due to the relatively high field-effect mobility in several organic materials. In these organic semiconductors, however, researchers have not established a reliable method of doping at a very low density level, although this has been crucial for the technological development of inorganic semiconductors. In the field-effect device structures, the conduction channel exists at the interface between organic thin films and SiO2 gate insulators. Here, we discuss a new technique that enables us to control the charge density in the channel by using organosilane self-assembled monolayers (SAMs) on SiO2 gate insulators. SAMs with fluorine and amino groups have been shown to accumulate holes and electrons, respectively, in the transistor channel: these properties are understood in terms of the effects of electric dipoles of the SAMs molecules, and weak charge transfer between organic films and SAMs.