Piezoelectric nanogenerators based on piezoelectric nanocomposites have attracted much interest in recent decades owing to their excellent piezoelectric properties and application in self-powered systems and wearable sensors. As a promising piezoelectric ceramic filler in composite-based generators, one-dimensional (1D) piezoelectric nanowires were filled into a polymer matrix to enhance its dielectric and piezoelectric properties. In this paper, flexible PVDF-TrFE composite films containing highly aligned Ba0.85Ca0.15Ti0.9Zr0.1O3 (BCZT) nanowires (NWs) have been manufactured via a direct-ink writing method. The effect of BCZT NW content on the dielectric, ferroelectric, and piezoelectric properties was investigated using multiphysics modeling and detailed experiments. An optimum composite composition was discovered, and the piezoelectric composite film with 15 wt % BCZT NWs possessed the highest energy harvesting figure of merit of 5.3 × 10-12 m2/N. Interdigital electrodes were combined with the composite to fabricate a patterned piezoelectric nanogenerator, where the piezoelectric nanogenerator can produce an open-circuit output voltage of 17 V, and the maximum output power density could reach 5.6 μW/cm2. This work provides opportunities for the optimization and fabrication of piezoelectric materials for energy-harvesting and sensing applications.