High-mobility organic field-effect transistors (OFETs) are the basic units for a variety of high-performance electronic applications. Here, we review recent progress in controlling molecular packing and crystal growth in high-mobility, small molecular organic FETs. Strategies to tune molecular packing of organic semiconductors and their impact on charge transport are described. Methods for the controlled growth of single-crystal organic semiconductors required for large-area device construction are reviewed. Furthermore, the advantages, limitations, and potential of these methods are also discussed.