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The charge carrier mobility of organic field‐effect transistors (OFETs) has been remarkably improved through several engineering approaches and techniques by targeting pivotal parts. Herein, an ultrathin perovskite channel layer that boosts the field‐effect mobility of conjugated polymer OFETs by forming perovskite‐conjugated polymer hybrid semiconducting channel is introduced. The optimized lead‐iodide‐based perovskite‐conjugated polymer hybrid channel transistors show enhanced hole mobility of over 4 cm2 V–1 s–1 (average = 2.10 cm2 V–1 s–1) with high reproducibility using a benchmark poly(3‐hexylthiophene) (P3HT) polymer and employing high‐k fluorinated polymer dielectrics. A significant hole carrier mobility enhancement of ≈200–400% in benzo[1,2‐b:4,5:b′]dithiophene (BDT)‐based conjugated polymers is also demonstrated by exploring certain interactive groups with perovskite. This significant enhancement in the transistor performance is attributed to the increased charge carrier density in the hybrid semiconducting channel and the perovskite–polymer interactions. The findings of this paper demonstrate an exceptional engineering approach for carrier mobility enhancement in hybrid perovskite‐conjugated‐polymer‐based electronic devices.

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In emerging perovskite transistors, interfacial engineering is pivotal for modulating the effective charge carrier transport; however, gate dielectric layer and its interface remain unexplored owing to the limited chemical stability of perovskites. Here, we propose an interfacial functionalization with a conjugated polymer to allow the use of high capacitance electrolyte dielectric in top-gate perovskite transistors. This multifunctional approach, exploiting orthogonal solution-processed polymers, enables blocking of chemical diffusion during the deposition of the dielectric, allows passivation of defects on the perovskite surface, results in air stability enhancement, and boosts mobility via the formation perovskite-polymer hybrid channels. The optimized conjugated polymer-capped lead iodide perovskite transistors showed a remarkable hole mobility of over 30 cm2 V–1 s–1 at ≤ 2 V. This result demonstrated the possibility of realizing high mobility through interfacial functionalization of perovskites in transistor applications.