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.