Organic field-effect transistors have received much attention in the area of low cost, large area, flexible, and printable electronic devices. Lots of efforts have been devoted to achieve comparable device performance with high charge carrier mobility and good air stability. Meanwhile, in order to reduce the fabrication costs, simple fabrication conditions such as the printing techniques have been frequently used. Apart from device optimization, developing novel organic semiconductor materials and using thin-film alignment techniques are other ways to achieve high-performance devices and functional device applications. It is expected that by combining proper organic semiconductor materials and appropriate fabrication techniques, high-performance devices for various applications could be obtained. In this chapter, the organic field-effect transistor in terms of device physics, organic materials, device process, and various thin-film alignment techniques will be discussed.