Currently, organic semiconductors (OSs) are widely used as active components in practical devices related to energy storage and conversion, optoelectronics, catalysis, and biological sensors, etc. To satisfy the actual requirements of different types of devices, chemical structure design and self‐assembly process control have been synergistically performed. The morphology and other basic properties of multiscale OS components are governed on a broad scale from nanometers to macroscopic micrometers. Herein, the up‐to‐date design strategies for fabricating multiscale OSs are comprehensively reviewed. Related representative works are introduced, applications in practical devices are discussed, and future research directions are presented. Design strategies combining the advances in organic synthetic chemistry and supramolecular assembly technology perform an integral role in the development of a new generation of multiscale OSs.