the amorphous silicon benchmark of 1 cm 2 Vs −1 , application of organic FETs in displays and sensors have now become a reality. Organic FETs differ from metal oxide semiconductor FET (MOSFET) in several ways; most organic FETs operate in the accumulation region compared to the inversion operating region of MOSFETs. The metal-semiconductor and the semiconductor-dielectric interfaces play a vital role in charge transport properties. In particular, the dielectric interface is notorious for charge trapping. As a result, achieving intrinsic transport in the organic semiconductor layer in FET architectures is very challenging. Using the same organic semiconductor film (either evaporated or solution processed) but different dielectric layers may yield order of magnitude differences in FET carrier mobilities. On the other hand, ultrapure organic single crystals such as rubrene, grown from vapor phase, have shown intrinsic FET mobilities higher than 20 cm 2 Vs −1 . [2] Since the charge accumulation is directly proportional to the dielectric capacitance (C), where; κ being the dielectric constant, ε 0 the permittivity of free space, A the area of the capacitor, and d the thickness of the dielectric, a high value of the dielectric capacitance is required for lowering the operating voltage of FETs. Low-operating voltage FETs, therefore, demand high κ dielectrics, which are more difficult to achieve with polymeric materials compared to inorganic dielectric materials due to their inherently low κ values. Facile methods of preparing polymer dielectrics by appropriate choice of solvents result in thin (well below 100 nm) and pinhole-free films for low-operating voltage FETs. [3,4] Polymer ferroelectrics with higher values of κ compared to non-ferroelectric polymers allow an alternate route toward boosting the capacitance values in FETs. Poly(vinylidene fluoride) (PVDF) ferroelectric polymer and its copolymer such as PVDF trifluorethylene (PVDF-TrFE) with κ > 8 at room temperature have been extensively used in memory and pressure sensing applications. [5][6][7][8][9] Naturally, such dielectrics also provide a route toward low-operating voltage FETs. The vast range of work has utilized PVDF and its copolymers as a gate dielectric in organic FETs. [10][11][12][13] Design of PVDF with carbon quantum dots has opened applications in nanogenerators where the mechanical energy may be efficiently converted to electricity. [14] More recently, PVDF copolymers have been used with charge-modulated organic FETs for multimodal Polymer ferroelectrics are playing an increasingly active role in flexible memory application and wearable electronics. The relaxor ferroelectric dielectric, poly(vinylidene fluoride trifluorethylene (PVDF-TrFE), although vastly used in organic field-effect transistors (FETs), has issues with gate leakage current especially when the film thickness is below 500 nm. This work demonstrates a novel method of selective poling the dielectric layer. By using solutionprocessed 6,13-bis(triisopropylsilylethynyl)pentacene (TIPS-p...