Achieving high performance in piezoactuators at extremely low temperatures is challenging and restricts the operating temperature range of devices in practical applications. In this study, 0.5 Pb(Ni1/3Nb2/3)O3-(0.5−x)PbTiO3-xPbZrO3+0.1 wt% MnCO3 bulk ceramics demonstrated a high piezoelectric strain coefficient of d33* = 1095 p.m./V at 1 kV/mm. Using a tape casting method, multilayer piezoactuators with a thickness of 48 μm and 32 active layers were prepared, and these devices exhibited high active strain (0.122%, 2.5 kV/mm) and total strain (0.085%, 2.5 kV/mm). The temperature-insensitive strain response was acquired at x = 0.15, with a variation of approximately 10% over the range from −100 to 110 °C, which surpassed the stability of current commercial PZT actuators. These results demonstrate that PZT-PNN multilayer piezoactuators promise to meet the requirements of high-performance devices and have potential for applications in harsh environmental conditions.