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Although solution processing has been hailed as a more industrially relevant route for the deposition of organic semiconductors to be used in devices, the quality and performance of solution-deposited thin films of these materials have not been able to reach that of vapor-grown single crystals until recently. Single crystals and single-crystalline films benefit from the absence of grain boundaries and the reduction of crystalline defects that impede effective charge transport through the solid. Although solution-phase deposition techniques for high-quality single-crystal growth have been reported, high-throughput, large-area deposition methods for single-crystalline films remain challenging. However, a shift toward this direction has emerged in recent years and has produced a diversity of techniques to grow, deposit, and pattern organic semiconductor single crystals and thin films. In this review, we survey the physical basis for a variety of solution-based single-crystal growth and deposition methods and discuss their advantages and shortcomings in the hopes of inspiring new ways to approach these challenges. [ABSTRACT FROM AUTHOR]