Developing self-powered and flexible optoelectronic sensors with high responsivity and speed is crucial for modern applications, motivating continuous efforts to enhance their performance. Flexo-phototronics is a less-explored but promising technique to elevate the performance of optoelectronics. Therefore, this work addresses the potential of utilizing the flexo-phototronic effect to enhance the performance of a flexible and self-powered ultraviolet photodetector (UV PD) based on ZnAl:LDH (layered double hydroxides) nanosheets (Ns)/NiO heterostructure. The vertically oriented ZnAl:LDH Ns are synthesized via a simple method involving the immersion of a sputtered 10% Al-doped ZnO thin film in deionized water at room ambient conditions. The fabricated PD exhibits an impressive response to 365 nm UV light, with high sensitivity in the order of 103. The device's photocurrent and responsivity are significantly enhanced by the flexo-phototronic effect, attributed to the flexoelectric properties of ZnAl:LDH Ns. Specifically, applying an inhomogeneous tensile strain of 2% boosted the device responsivity by 57.1% and improved its operational speed. Furthermore, a working model revealing the altered energy-band structure is demonstrated to elucidate the flexo-phototronic-induced boost in the photoresponse. The PD also demonstrated a sustainable performance under severe bending cycles, underlining the good flexibility of the device. The results presented in this study demonstrate a self-powered and flexible UV PD and provide a viable approach to augment the performance of optoelectronics through the flexo-phototronic effect.