Solution-Processed, Large-Area Two-Dimensional Organic Single-Crystalline Films: Strategies, Mechanisms, and Applications.

π-conjugated two-dimensional (2D) organic single-crystalline films (OSCFs) hold great promise for next-generation organic electronics, thanks to their ultrathin morphology, absence of grain boundaries, long-range molecular order, and excellent charge transport properties. Among various fabrication strategies, solution-processed approaches have garnered significant attention due to their ability to regulate nucleation and growth dynamics, thereby enabling the scalable fabrication of large-area, high-quality, 2D OSCFs. This review systematically examines the key parameters governing the large-area growth of 2D OSCFs, with a focused discussion on the advantages and limitations of representative solution-processed approaches. Recent breakthroughs in 2D OSCF-based field-effect transistors are highlighted along with their emerging applications in integrated organic circuits. Finally, the key challenges and further perspectives are outlined in order to promote the future development of the 2D OSCFs in next-generation high-performance organic electronic devices.