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The study of monolayer organic field‐effect transistors (MOFETs) provides an effective way to investigate the intrinsic charge transport of semiconductors. To date, the research based on organic monolayers on polymeric dielectrics lays far behind that on inorganic dielectrics and the realization of a bulk‐like carrier mobility on pure polymer dielectrics is still a formidable challenge for MOFETs. Herein, a quasi‐monolayer coverage of pentacene film with orthorhombic phase is grown on the poly (amic acid) (PAA) dielectric layer. More significantly, charge density redistribution occurs at the interface between the pentacene and PAA caused by electron transfer from pentacene to the PAA dielectric layer, which is verified by theoretical simulations and experiments. As a consequence, an enhanced hole accumulation layer is formed and pentacene‐based MOFETs on pure polymer dielectrics exhibit bulk‐like carrier mobilities of up to 13.7 cm2 V−1 s−1 from the saturation region at low VGS, 9.1 cm2 V−1 s−1 at high VGS and 7.6 cm2 V−1 s−1 from the linear region, which presents one of the best results of previously reported MOFETs so far and indicates that the monolayer semiconductor growing on pure polymer dielectric could produce highly efficient charge transport. [ABSTRACT FROM AUTHOR]