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The first GaS nanosheet-based photodetectors are demonstrated on both mechanically rigid and flexible substrates. Highly crystalline, exfoliated GaS nanosheets are promising for optoelectronics due to strong absorption in the UV–visible wavelength region. Photocurrent measurements of GaS nanosheet photodetectors made on SiO₂/Si substrates and flexible polyethylene terephthalate (PET) substrates exhibit a photoresponsivity at 254 nm up to 4.2 AW^–1 and 19.2 AW^–1, respectively, which exceeds that of graphene, MoS₂, or other 2D material-based devices. Additionally, the linear dynamic range of the devices on SiO₂/Si and PET substrates are 97.7 dBでしべる and 78.73 dBでしべる, respectively. Both surpass that of currently exploited InGaAs photodetectors (66 dBでしべる). Theoretical modeling of the electronic structures indicates that the reduction of the effective mass at the valence band maximum (VBM) with decreasing sheet …