Advances in Single‐Crystal Films: Synergistic Insights from Perovskites and Organic Molecules for High‐Performance Optoelectronics

Abstract Semiconductor single‐crystal thin films are crucial for the advancement of high‐performance optoelectronic devices. Despite significant progress in fabricating perovskite and organic single‐crystal films, interdisciplinary insights between these domains remain unexplored. This review aims to bridge this gap by summarizing recent advances in fabrication strategies for perovskite and organic molecular single‐crystal films. Five preparation methods—solution‐phase epitaxy, solid‐phase epitaxy, meniscus‐induced crystallization, antisolvent‐induced crystallization, and space‐confined growth—are analyzed with a focus on their principles, functional properties, and distinct advantages. By comparing these approaches across material systems, this review identifies transferable insights that can drive the development of large‐scale, high‐quality single‐crystal films. Furthermore, the optoelectronic applications of these films are explored, including solar cells, photodetectors, light‐emitting devices, and transistors, while addressing challenges such as scalability, defect control, and integration. This work highlights the importance of cross‐disciplinary innovation and provides an effective pathway for integrating perovskite and organic molecular processing to advance the next generation of single‐crystal film technologies.