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The disordered chain arrangement of polymer dielectrics has complex both internal and external effects on system performance, which generally stimulates the weak acquisition and grain boundaries of vapor‐deposited organic small molecule films (VDOSMFs) with thermally activated charge transport. As a result, achieving "band‐like" transmission of VDOSMs on polymer dielectrics is attempting to prove to be a major challenge. Three types of bi‐polymer dielectrics are developed to modulate charge transport from thermally activated mode to "band‐like" transport at the interfacial level. The bottom consisting of a polyimide layer is critical to interfacial modulation, which shows the selectively binding capability with up‐dielectric layers to realize the modulation of charge transport, as corroborated by interface characterization and density functional‐based tight‐binding calculation. The findings provide an effective strategy for modulating the charge transport through polymer dielectric engineering and also recommend a podium to further comprehend the electrical characteristics of small molecules in organic thin‐film transistors. [ABSTRACT FROM AUTHOR]

Molecule design of organic semiconductors (OSCs) for eliminating photoresponse and maintaining high charge mobility concurrently is beneficial to realize intrinsically photostable and high‐performance organic field‐effect transistors (OFETs), which has never been reported. Here, a novel organic semiconductor TFP‐TT‐TPA with a centrosymmetric structure is synthesized. Remarkably, OFETs with TFP‐TT‐TPA show negligible photoresponse under light intensity up to 170.4 mW cm−2 (higher than sunlight intensity, about 138 mW cm−2), which ensures that the devices can work stably under sunlight. Through the single‐crystal structure and exciton dynamics analysis, it is found that the specific structure design can make strong intermolecular D–A interaction that occurs in the aggregate state, which facilitates the process of exciton quenching and thus enables the photostable OFETs. This study provides a new strategy for the design of organic semiconductors with intrinsic photostability and the construction of photostable organic optoelectronic devices for applications in light environment. [ABSTRACT FROM AUTHOR]