Flexible nanocomposite generators based on piezoelectric nanoparticles (NPs)-polymeric matrix have been attracted attention as the energy harvesting device converted the electricity from the mechanical deformations. To enhance the piezo-potential difference introduced inside the piezoelectric nanocomposite, one-dimensional nanostructures such as CNTs, copper nanorods, and Ag nanowires (NWs) should be used inevitably as a dispersing agent for achieving well-distributed piezoelectric nanoparticles in an elastomer. These non-piezoelectric additives showed versatile roles; however, their toxicity to living organism has been an obstacle to realize the bio-eco-friendly flexible energy harvesters. Replacing them with piezoelectric NWs with non-toxic can be a challengeable approach to achieve not only the original purposes of additives but also the improvement of output performance. Here, we synthesized well-crystallized BaTiO3 spherical and acicular NPs via a simple hydrothermal reaction and the two-step hydrothermal reactions, respectively and produced piezoelectric nanocomposite made of piezoelectric BaTiO3 NPs and NWs without toxic dispersion enhancers. Output performance of the fabricated flexible energy harvesters with varying the composition of NPs and NWs were investigated by the well-optimized measurement system during the periodical bending and unbending. A nanocomposite-based energy harvester with 4:1 wt ratio generated the maximum open-circuit voltage and short-circuit current of 60 V and 1.1 mu A, respectively.