[en] Organic semiconductors, which include a diverse range of carbon-based small molecules and polymers with interesting optoelectronic properties, offer many advantages over conventional inorganic semiconductors such as silicon and are growing in importance in electronic applications. Although these materials are now the basis of a lucrative industry in electronic displays, many promising applications such as photovoltaics remain largely untapped. One major impediment to more rapid development and widespread adoption of organic semiconductor technologies is that device performance is not easily predicted from the chemical structure of the constituent molecules. Fundamentally, this is because organic semiconductor molecules, unlike inorganic materials, interact by weak non-covalent forces, resulting in significant structural disorder that can strongly impact electronic properties. Nevertheless, directional forces between generally anisotropic organic-semiconductor molecules, combined with translational symmetry breaking at interfaces, can be exploited to control supramolecular order and consequent electronic properties in these materials. This review surveys recent advances in understanding of supramolecular assembly at organic-semiconductor interfaces and its impact on device properties in a number of applications, including transistors, light-emitting diodes, and photovoltaics. Recent progress and challenges in computer simulations of supramolecular assembly and orientational anisotropy at these interfaces is also addressed. (topical review)