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Polymer-based gate dielectrics have received growing attention due to their important role in field-effect transistors (OFETs). This review article aims to present the recent progress of polymer dielectrics for high-performance OFET applications. We first discuss the requirements for polymer dielectrics in tailoring the overall performance of OFETs from the perspective of both bulk material properties and surface characteristics of the polymers. On this basis, we introduce the design strategies and desired processing techniques of polymer dielectrics for optimizing the charge transport and stabilizing the operation of OFETs. Then, we highlight the recent advances in polymer-based dielectrics by classifying and comparing different categories of polymeric materials as well as polymer nanocomposites, and focus is also given to elucidating the critical relationships between polymer structures, gate dielectric properties and OFET performance. Finally, a perspective of future research directions and challenges for polymer dielectrics is provided.

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