A new thin-film coating process, scanning corona-discharge coating (SCDC), to fabricate ultrathin tri-isopropylsilylethynyl pentacene (TIPS-PEN)/amorphous-polymer blend layers suitable for high-performance, bottom-gate, organic thin-film transistors (OTFTs) is described. The method is based on utilizing the electrodynamic flow of gas molecules that are corona-discharged at a sharp metallic tip under a high voltage and subsequently directed towards a bottom electrode. With the static movement of the bottom electrode, on which a blend solution of TIPS-PEN and an amorphous polymer is deposited, SCDC provides an efficient route to produce uniform blend films with thicknesses of less than one hundred nanometers, in which the TIPS-PEN and the amorphous polymer are vertically phase-separated into a bilayered structure with a single-crystalline nature of the TIPS-PEN. A bottom-gate field-effect transistor with a blend layer of TIPS-PEN/polystyrene (PS) (90/10 wt%) operated at ambient conditions, for example, indeed exhibits a highly reliable device performance with a field-effect mobility of approximately 0.23 cm2 V−1 s−1: two orders of magnitude greater than that of a spin-coated blend film. SCDC also turns out to be applicable to other amorphous polymers, such as poly(α-methyl styrene) and poly(methyl methacrylate) and, readily combined with the conventional transfer-printing technique, gives rise to micropatterned arrays of TIPS-PEN/polymer films.