By virtue of the biocompatibility, environmental benignity, and sustainability, as well as low cost of keratin protein's source herein, we report its application as a gate dielectric material for organic electronic devices. Keratin protein, which is a biodegradable material was directly extracted from poultry chicken feathers (CFs). Solution-processed regioregular poly(3-hexylthiophene) (P3HT) organic thin film transistors (OTFTs) with keratin dielectric thin film exhibited enhanced charge mobility of 2.293 × 10−3 cm2 V−1 s−1 (saturation regime), high on-off current ratio of 105 and low threshold voltage, -1V as compared to conventional SiO2 dielectric. All the fabrication processes were performed below 100 °C. A detailed semiconductor-dielectric interface study has revealed that the high content of β-sheet structure in keratin protein has guided the P3HT polymer chains, through supramolecular forces of interaction to form 2D nanoribbons of large crystallite size (150 nm) over keratin thin film. This has led to the reduced trapping sites at the semiconductor/dielectric interface and hence the enhanced electrical performance of OTFTs was observed. Atomic force microscopy (AFM) and Grazing Incidence X-ray diffraction (GI-XRD) study was further employed to explore the mechanism of formation of 2D nanoribbons of P3HT. The primary and secondary structure of keratin protein as analyzed by AFM, Transmission electron microscopy (TEM) and Fourier transform spectroscopy (FTIR) is also provided in this study. The water compatible nature of keratin has helped to overcome the common issue of dielectric layer washing that occurs mostly during fabrication of OTFTs by sol-gel method. The biodegradable nature of keratin protein has also been demonstrated here by providing it as feed to fishes in an aquarium.