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The self-powered PVP-Co@C nanofibers/n-GaAs heterojunction photodetector (HJPD) was fabricated by electrospinning of the nanofibers onto GaAs. An excellent rectification ratio of 6.60 × 106 was obtained from I – V measurements of the device in the dark. The I – V measurements of the fabricated device under 365 nm, 395 nm and 850 nm lights, as well as I – V measurements in visible light depending on the light intensity, were performed. The HJPD demonstrated excellent photodetection performance in terms of a good responsivity of ∼225 mA W−1 (at −1.72 V) and at zero bias, an impressive detectivity of 6.28 × 1012 Jones, and a high on/off ratio of 8.38 × 105, all at 365 nm wavelength. In addition, the maximum external quantum efficiency and NPDR values were 3495% (V = −1.72 V) and 2.60 × 1010 W−1 (V = 0.0 V), respectively, while the minimum NEP value was ∼10−14 W.Hz−1/2 for 365 nm at V = 0.V volts. The HJPD also exhibited good long-term stability in air after 30 d without any encapsulation. [ABSTRACT FROM AUTHOR]