bandgap semiconductors, such as SiC, diamond, Ga 2 O 3 , GaN, ZnS, ZnO, or ZnSe, suffer from problems, such as low sensitivity, long response time, nonlinear photocurrent with incident optical power, and a complicated fabrication process. [3][4][5][6] In addition, the fabrication of a flexible or rollable UV photodetector with sufficient durability has not been reported, despite the great significance of sustainable mechanical flexibility for the sensor in wearable sensing systems.Many studies have been focused on developing efficient, flexible, and highly sensitive UV photodetectors from various nanostructured materials. As an emerging nanomaterial for effective flexible photodetectors, 2D nanomaterials have attracted considerable attention because of their unique properties, such as atomic-scale thickness, lightweight, and flexibility. [8,9] One representative 2D nanomaterial, layered double hydroxides (LDHs), has received considerable attention owing to their novel optical, electrical, structural, and electrochemical properties. [10][11][12][13][14] LDHs are functional clay composed of an interlayer anion and a host layer that is positively charged in a layer-by-layer structure. The general chemical composition of LDHs can be described in the formula [M 2+(1-α) N 3+ (OH) 2 ] α + [A n− ] α/n •mH 2 O, where M 2+ is the divalent cation (e.g.
