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In this study, we fabricated flexible organic field-effect transistors (OFETs) (bottom-gate and top-contact architecture) based on the blend film composed of 6,13-bis(triisopropylsilylethynyl) pentacene (TIPS pentacene) as a π-conjugated small-molecule semiconductor and polystyrene (PS) as a polymer insulator. Blend solutions including both the TIPS pentacene and PS molecules were electrosprayed onto bottom-gate electrodes which were patterned on polyethylene naphthalate films. The devices exhibited superior electrical characteristics due to well-defined vertical phase separation between the TIPS pentacene crystalline layer (top) and PS insulator (bottom). This study will contribute to a facile one-step printing process to produce high-performance flexible OFETs.