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In this paper, an amorphous Ga2O3 metal–semiconductor–metal photodetectors passivated by the organosilicon layer were reported. Due to the excellent passivation property of the passivation layer and the diffusion effect of hydrogen, the responsivity of Ga2O3 photodetectors was improved effectively, while the dark state current is basically unchanged. The results of x-ray photoelectron spectroscopy have proved that the amount of oxygen vacancy near the interface between organosilicon and Ga2O3 layer has been passivated and the surface chemisorption was suppressed via capping a foreign layer after the deposition of organosilicon passivation layer. The Ga2O3 photodetectors with organosilicon passivation layer exhibit a boosted performance, with a low dark current of 2.96 × 10−12 A, a responsivity of 11.82 A/W, and a specific detectivity of 9.01 × 1014 Jones. [ABSTRACT FROM AUTHOR]