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Visible-blind ultraviolet (UV) photodetectors have received a great deal of attention for realizing Internet of Things technologies as well as for monitoring the level of UV exposure to humans. Realizing next-generation flexible and visible-blind UV photodetectors requires development of new functional material systems with easy fabrication, selectively strong UV light absorption, environmental friendliness, and high stability regardless of ambient conditions. Herein, flexible visible-blind UV photodetectors are successfully fabricated on the basis of two-dimensional ZnAl-layered double hydroxide (LDH) nanosheets with scroll structures grown on flexible substrates. The ZnAl-LDH nanosheet scrolls exhibit highly resistive semiconducting properties with a band gap of 3.2 eV and work function of 3.64 eV. The photodetector based on the ZnAl-LDH shows photoresponse in the UV spectral range below 420 nm, indicating visible-blind spectral response. In addition, the UV photodetector shows a maximum responsivity of 17 mA/W under illumination with 365 nm light. Moreover, the flexible photodetector shows reproducible photoresponse even after 1000 bending cycles, which indicates the acceptable stability of the ZnAl-LDH nanosheet scrolls.