In recent years, organic semiconductor (OSC) ultrathin films and their solution-processed organic field-effect transistors (OFETs) have garnered attention for their high flexibility, light weight, solution processability, and tunable optoelectronic properties. These features make them promising candidates for next-generation optoelectronic applications. An ultrathin film typically refers to a film thickness of less than 10 nm, i.e., several molecular layers, which poses challenges for OSC materials and solution-processed methods. In this paper, first we introduce the carrier-transport regulation mechanism under ultrathin limits. Second, we summarize various solution-processed techniques for OSC ultrathin films and elucidate advances in their OFETs performance, such as enhanced or maintained mobilities, improved switching ratios, reduced threshold voltages, and minimized contact resistance. The relationship between the ultrathin-film thickness, microstructure of various OSCs (small molecules and polymers), and device performance is discussed. Third, we explore the recent application of OSC ultrathin-film-based OFETs, such as gas sensors, biosensors, photodetectors, and ferroelectric OFETs (Fe-OFETs). Finally, the conclusion is drawn, and the challenges and prospects of ultrathin OSC transistors are presented. Nowadays, research on ultrathin films is still in its early stages; further experience in precise film deposition control is crucial to advancing research and broadening the scope of applications for OSC ultrathin devices.
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