This work highlights recent literature dealing with the fabrication of field-effect transistors from the vacuum deposition of organic semiconductors. We pay special attention to recent advances in molecular design and specific ways that synthesis has been used to tune crystal packing, and thus charge transport, in organic semiconductors. This work also looks into the fundamental processes of nucleation and growth of organic semiconductors that are deposited by vacuum deposition. The parameters that affect the morphology of the corresponding films are discussed in detail. We also provide specific examples from a family of fluorene-thiophene containing oligomers that correlate the molecular structure to device performance.