A “33” mode (mechanical stress being in parallel to the electric dipole moment direction) piezoelectric lead zirconate titanate (PZT) multilayer stack-based piezoelectric flextensional energy harvester (PZT-Stacked-FEH) has been developed. Interdisciplinary approaches had been taken to increase the performance of the PZT-Stacked-FEH. First, an elastic flextensional frame for force amplification has been optimally designed to capture more mechanical energy with high energy transition efficiency into the PZT-Stacked-FEH. Second, a “33” mode piezoelectric PZT multilayer stack (PZT-Stack) was employed instead of “31” mode (stress being in perpendicular to the dipole moment direction) single layer piezoelectric component to increase mechanical to electrical energy conversion efficiency and to generate more electrical charges in order to improve energy storage efficiency. With these approaches, the PZT-Stacked-FEH demonstrates excellent performance: 1) a 19% of overall mechanical to electrical energy conversion efficiency was achieved, 2) 48.6 times more mechanical energy was transited into PZT-Stacked-FEH and 26.5 times more electrical power was generated than directly applying force to the PZT-stack, and 3) energy storage efficiency was significantly improved. In this paper, we are focusing on the investigations for the off-resonance mode performance of the PZT-Stacked-FEH through theoretical modeling, prototype development, and experimental studies. A prototype PZT-Stacked-FEH of weight 18 grams was able to generate 666 mW electrical power under 52 Nrms force at 250 Hz, which is much lower than the resonant frequency (936 Hz). At this condition, a 6,600 μF super-capacitor was charged from 0 to 7 V in 1.6 second, at an average rate of 100 mW. Furthermore, 70% of generated appear electrical powers were delivered to matched resistive loads in the investigated regime of frequencies. Finally, the experimental results matched well with theoretical predictions which verified the developed theoretical models.