Abstract: | Polymeric dielectrics play a key role in the realization of flexible organic electronics, especially for the fabrication of scalable device arrays and integrated circuits. Among a wide variety of polymeric dielectric materials, aromatic polyimides (PIs) are flexible, lightweight, and strongly resistant to high‐temperature processing and corrosive etchants and, therefore, have become promising candidates as gate dielectrics with good feasibility in manufacturing organic electronic devices. More significantly, the characteristics of PIs can be conveniently modulated by the design of their chemical structures. Herein, from the perspective of structure optimization and interface engineering, a brief overview of recent progress in PI‐based dielectrics for organic electronic devices and circuits is provided. Also, an outlook of future research directions and challenges for polyimide dielectric materials is presented. |