Flexible ultraviolet (UV) photodetectors have attracted extensive research interest due to their potential applications in personal UV monitoring, UV electronic eye, anti-UV gloves, and other wearable systems. In this study, we present a highly sensitive flexible UV photodetector based on an ultrathin GaAs layer that is produced using a metal−organic chemical vapor deposition method and epitaxial lift-off film transfer technology. Device performance analysis reveals that the photodetectors made of a 50 nm thick GaAs layer have excellent sensitivity to 365 nm light. Specifically, the responsivity, specific detectivity, and external quantum efficiency could reach as high as 99.01 A W −1 , 1.51 × 10 12 Jones, and 3.37 × 10 4 %, respectively, at −2 V bias voltage, which are comparable to many UV photodetectors made from conventional wide band gap semiconductors. Such outstanding UV response properties are related to the very high absorption coefficient for UV light and carrier mobility of an ultrathin GaAs film. Equally importantly, the mechanical flexibility resulting from reducing the film thickness allows the device to maintain its photoelectric properties even after more than 500 bending cycles. The totality of these results suggests that our flexible UV photodetectors have strong potential applications in future wearable devices.