This research utilizes waste heat energy as a sustainable energy source to enhance pyroelectric power output by combining pyroelectric nanogenerators with an external pulsed electric field. When the surface temperature of the pyroelectric body varies, applying different pulses of the external electric field results in maximum power accumulation. A novel power-generating experimental setup was developed to measure and compute pyroelectric power generation. A standard Fuji ceramic C-9 sample was used to generate pyroelectric energy in a 20 °C temperature range from 120 to 140 °C. The continuous temperature variation frequency was 0.05 Hz, and the pulsed electric field was applied when the temperature rose. Pulses of the electric field with widths of 10, 50, 100, and 200 ms were applied to the sample under different pulse amplitudes, and the amplitude of each pulse was 250, 500, 1000, or 1500 V/mm. The maximum power generated through the application of an external pulsed electric field under the above-mentioned conditions was evaluated. This system had the highest power density of 0.204 mJ cm−2 °C−1 kV−1. In addition, for the lowest input power, the maximum power generation condition was a 10 ms pulse width and an amplitude of 250 V mm−1 in the applied electric field. This state might power smart sensor modules, IoT devices, automobiles, and other waste heat energy applications. Nano-pulse electric field applications may reduce input power to its lowest level, dependent on net-producing power. Therefore, new researchers can use net-generation power efficiency to create a large-scale power source using multiple pyroelectric arrays.