The rising demand for efficient energy storage in flexible electronics is driving the search for materials that are well-suited for the fabrication of these devices. Layered Double Hydroxides (LDHs) stand out as a remarkable material with a layered structure that embodies exceptional electrochemical properties. In this study, both double-shelled and single-shelled NiFe-Layered Double Hydroxide (LDH) particles are prepared using spindle-shaped MIL-101(Fe) as the template. These NiFe-LDH particles are then utilized to develop a flexible energy storage device. Transmission electron microscopy(TEM) analysis revealed that the as-synthesized NiFe-LDH particles transformed into hollow single-shells from a double-shelled structure as the aging time increased, which significantly influenced the electrochemical performances. Despite the decreasing specific capacitance and energy density with longer etching times, the sample etched for 2 h (NiFe-LDH 2h) demonstrated the highest capacitance of 9.24 mF·cm⁻