Low-cost solution-shearing methods are highly desirable for deposition of organic semiconductor crystals over a large area. To enhance the rate of evaporation and deposition, elevated substrate temperature is commonly employed during shearing processes. However, the Marangoni flow induced by a temperature-dependent surface-tension gradient near the meniscus line shows negative effects on the deposited crystals and its electrical properties. In the current study, the Marangoni effect to improve the shearing process of 2,7-dioctyl[1]benzothieno[3,2-b][1]benzothiophene for organic field-effect transistor (OFET) applications is utilized and regulated. By modifying the gradient of surface tension with different combinations of solvents, the mass transport of molecules is much more favorable, which largely enhances the deposition rate, reduces organic crystal thickness, enlarges grain sizes, and improves coverage. The average and highest mobility of OFETs can be increased up to 13.7 and 16 cm 2 V −1 s −1 . This method provides a simple deposition approach on a large scale, which allows to further fabricate large-area circuits, flexible displays, or bioimplantable sensors.