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Flexible solution-processed polymer thin-film transistors (PTFTs) with a low band-gap (LBG) donor–acceptor (D–A) conjugated polymer as the active layer and electrochemically oxidized alumina (AlOx:Nd) as the gate insulator are fabricated on polyethylene naphthalate (PEN) substrates. The AlOx:Nd insulator exhibits excellent insulating properties with low leakage current, a high dielectric constant and a high breakdown field. To improve the interface coupling between the polymer active layer and the AlOx:Nd insulator, the AlOx:Nd insulator is treated with octadecyl-phosphonic acid (ODPA), forming self-assembled monolayers (SAMs) on the surface, and great improvement in TFT performance with the highest mobility of 2.88 cm2 V−1 s−1 is attained. The performance improvement is attributed to the smoother surface and lower surface energy of the ODPA-treated AlOx:Nd compared to those of bare AlOx:Nd. In …