Gas–Solid Interface‐Assisted Growth of Organic Semiconductor Single Crystals: Dimensions, Structures, Mechanisms, and Applications

Organic semiconductor single crystals (OSSCs) represent a critical materials platform for pushing the performance limits of organic optoelectronic devices, owing to their structural perfection, absence of grain boundaries and ultralow trap densities. Among existing growth methods, gas–solid interface‐assisted growth strategy stands out, due to its superior advantages in controlling the dimension, morphology, structure, and orientation of OSSCs. Recent breakthroughs demonstrate that precise manipulation of nucleation and growth dynamics, through tailored temperature, carrier gas engineering, interface modification and molecular component optimization, enables the reproducible preparation of high‐quality OSSCs at gas–solid interface. This review provides a comprehensive overview of the fundamental principles and state‐of‐the‐art gas–solid interface‐assisted growth strategies. It critically examines the relationship between growth parameters and resulting crystal properties, highlights representative high‐performance devices based on such crystals, and outlines key challenges and outlooks for advancing this approach toward high‐performance organic optoelectronics.