A unified approach of directional solvent vapor annealing for crystal alignment in solution-processed organic semiconductors is proposed. Highly crystalline molecular self-assembly of the drop-cast technique is further enhanced by postprocessing scheme of the solvent vapor annealing with additional benefit of alignment of the crystalline domains. In this technique, a mixture of carrier gas and solvent vapors are made to flow in a certain direction and in the close proximity of the surface of the substrates carrying the solution. Flow of the carrier gas imparts directionality to the semiconducting crystalline ribbons, whereas the influx of the solvent vapors improves the crystalline order in the semiconducting film. The flow rate of the carrier gas and the position of the substrate in the interaction chamber are the primary regulating factors, which have the ability to provide a semiconducting layer with a well-aligned and interconnected assembly of long ribbons. These favorable film properties further materialize in the form of electrical performance of the corresponding field-effect transistors. The versatility of this technique makes it a viable alternative for the solution processing of organic semiconductors. © 2017 American Chemical Society.