We fabricated an organic thin-film transistor (OTFT) using an all-step solution process. The printed layers, in which the electrode (silver), dielectric layer (BaTiO3–PMMA), source–drain layer, and semiconductor 6,13-Bis(triisopropylsilylethynyl)pentacene(TIPS–pentacene), were optimized using roll-to-roll, an inkjet printer, and drop-casting. After coating the source–drain layer, we applied ultraviolet (UV)–ozone and self-assembled monolayer (SAM) treatments to the composite layer. The OTFTs treated with the UV–ozone and SAM treatments were found to exhibit excellent performance and good properties in comparison to silicon-based OTFTs.