Recent studies have focused on the development of efficient, flexible, and highly sensitive ultraviolet photodetectors (UV PDs) with various wide band-gap materials. In the present study, the application of environmentally friendly zinc−aluminum layered double hydroxide (ZnAl−CO 3 :LDH) is demonstrated for a high-performance, flexible UV PD. The vertically oriented ZnAl:LDH nanosheets (ZnAl:LDH Ns) are facilely synthesized by dipping the sputtered 10 wt % aluminum-doped zinc oxide thin films in deionized water at room temperature. Without passivation, the UV PDs exhibit an exceptional light-to-dark current ratio of 10 4 and a responsivity of ∼34.7 mA/W at a bias of 1 V. Moreover, the spectral responsivity and detectivity are enhanced to ∼148.3 mA/W and 2.5 × 10 12 Jones, respectively, by passivating the ZnAl:LDH Ns with polydimethylsiloxane (PDMS), thus making the device suitable for application in UV detectors. In addition, the ambient atmosphere effect on PD performance, which elucidates the clear understanding of the PD working mechanism, is also investigated. The passivation of the Ns by PDMS also helps to enhance the mechanical robustness and long-term stability of the PD. The methodology demonstrated herein highlights the potential of the ZnAl:LDH material in realizing the next generation of flexible UV PDs.