| Summary: | The fabrication of high-performance Organic Phototransistors (OPTs) by depositing Al-islands atop Poly(3-hexylthiophene) (P3HT) thin film coated using the unidirectional floating-film transfer method (UFTM) has been realized. Further, the effect of Al-island thickness on the OPTs’ performance has been intensively investigated using X-ray photoelectron spectroscopy, X-ray Diffraction, Atomic force microscopy and UV-Vis spectroscopy analysis. Under the optimized conditions, OPTs’ mobility and on–off ratio were found to be 2 × 10<sup>−2</sup> cm<sup>2</sup> V<sup>−1</sup> s<sup>−1</sup> and 3 × 10<sup>4</sup>, respectively. Further, the device exhibited high photosensitivity of 10<sup>5</sup>, responsivity of 339 A/W, detectivity of 3 × 10<sup>14</sup> Jones, and external quantum efficiency of 7.8 × 10<sup>3</sup>% when illuminated with a 525 nm LED laser (0.3 mW/cm<sup>2</sup>).
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