Low cost and ecological printing methods for mass production of thin, light, flexible electronic devices incorporating organic semiconductors are key to the further integration of electronics into everyday life. In this light, we have developed an all-solution fabrication process for plastic electronics devices, in which all components of devices spontaneously assemble with desired geometry. By formation of surface molecular template composed of self-assembled monolayers, complete arrays of organic field-effect transistors including gate electrodes, source and drain electrodes, and organic semiconductor layers have been patterned from solution phase with excellent operational characteristics on a plastic substrate. This bottom-up method of device fabrication, in which the functional properties of molecules are utilized for their spontaneous assembly, may become a core technology for plastic electronics. In this paper, we describe the principles of the surface-selective deposition technique and its application to electronic device production processes.