Quenching has recently demonstrated its efficacy in elevating the ferroelectric to relaxor phase transition temperature (TFR) in 0.94Na0.5Bi0.5TiO3-0.06BaTiO3 (NBT-6BT). Consequently, the current investigation comprehensively examines the pyroelectric properties of quenched NBT-6BT. The pyroelectric coefficient is measured using the Byer-Roundy method, incorporating a strategic approach to mitigate the risk of overestimation by implementing cyclic heating and cooling. Quenching enhances the depolarization temperature (Td) by approximately 40 °C, quantified through the temperature-dependent pyroelectric current density (Ip). The maximum pyroelectric current (52nA) and voltage (200V) responses to thermal cycling (15s heating/cooling) were observed in quenched NBT-6BT. The voltage sensitivity figures of merit were equivalent for both furnace-cooled and quenched NBT-6BT. The assessment of pyroelectric energy storage involved charging a 48 nF capacitor in 180s, resulting in a maximum voltage of 38V. The outcomes strongly endorse the quenched NBT-6BT as an efficient pyroelectric material, showcasing promising attributes for applications in sensing and energy harvesting across a broad temperature range.