Fabrication of organic thin-film transistors (OTFTs) via high throughput solution process routes have attracted extensive attention. Herein, we report a simple one-step coating method for vertical phase separation of the poly(3-hexylthiophene-2,5-diyl) (P3HT) and poly(methyl methacrylate) (PMMA) blends as semiconducting and dielectric layers in OTFTs. These OTFTs can be used as phototransistors for ultraviolet (UV) light detection, where the phototransistors exhibited great photosensitivity of 597.6 mA/W and detectivity of 4.25 × 1010 Jones under 1 mW/cm2 UV light intensity. Studies of the electrical properties in these phototransistors suggested that optimized P3HT contents in the blend film can facilitate the improvement of film morphology, and therefore form optimized vertical phase separation of the PMMA and P3HT. These results indicate that the simple one-step fabrication method creates possibilities for realizing high throughput phototransistors with great photosensitivity.