Composite-based piezoelectric devices are extensively studied to develop sustainable power supply and selfpowered devices owing to their excellent mechanical durability and output performance. In this study, we design a leadfree piezoelectric nanocomposite utilizing (Ba<sub>0.85</sub>Ca<sub>0.15</sub>)(Ti<sub>0.9</sub>Zr<sub>0.1</sub>)O<sub>3</sub> (BCTZ) nanomaterials for realizing highly flexible energy harvesters. To improve the output performance of the devices, we incorporate porous BCTZ nanowires (NWs) into the nanoparticle (NP)-based piezoelectric nanocomposite. BCTZ NPs and NWs are synthesized through the solidstate reaction and sol-gel-based electrospinning, respectively; subsequently, they are dispersed inside a polyimide matrix. The output performance of the energy harvesters is measured using an optimized measurement system during repetitive mechanical deformation by varying the composition of the NPs and NWs. A nanocomposite-based energy harvester with 4:1 weight ratio generates the maximum open-circuit voltage and short-circuit current of 0.83 V and 0.28 A, respectively. In this study, self-powered devices are constructed with enhanced output performance by using piezoelectric energy harvesting for application in flexible and wearable devices.