In organic field-effect transistors, the first few molecular layers at the semiconductor/dielectric interface are regarded as the active channel for charge transport; thus, great efforts have been devoted to the modification and optimization of molecular packing at such interfaces. Here, we report organic monolayers with large-area uniformity and high crystallinity deposited by an antisolvent-assisted spin-coating method acting as the templating layers between the dielectric and thermally evaporated semiconducting layers. The predeposited crystalline monolayers significantly enhance the film crystallinity of upper layers and the overall performance of transistors using these hybrid-deposited semiconducting films, showing a high carrier mobility up to 11.3 cm2 V-1 s-1. Additionally, patterned transistor arrays composed of the templating monolayers are fabricated, yielding an average mobility of 7.7 cm2 V-1 s-1. This work demonstrates a promising method for fabricating low-cost, high-performance, and large-area organic electronics.