The search for low-cost, large-area, flexible devices has led to a remarkable increase in the research and development of organic semiconductors, which serve as one of the most important components for organic field-effect transistors (OFETs). In the current review, we highlight deposition techniques that offer precise control over the location or in-plane orientation of organic semiconductors. We focus on various vapor- and solution-processing techniques for patterning organic single crystals in desired locations. Furthermore, the alignment of organic semiconductors via different methods relying on mechanical forces, alignment layers, epitaxial growth, and external magnetic and electric fields are surveyed. The advantages, limitations, and applications of these techniques in OFETs are also discussed.