AbstractHfAlO film‐based ferroelectric memory is a strong contender for the next‐generation nonvolatile memories. However, the remanent polarization intensity of HfAlO films is small compared to other Hf‐based ferroelectric films at low annealing temperatures. In order to further improve the remnant polarization of the device, the ferroelectric memory with metal‐ferroelectric‐metal structure using ZrO2 as the regulating layer (RL) is designed and fabricated. Experimental results show that the device with the ZrO2 regulating layer exhibits triple enhancement, which may be due to the fact that ZrO2 RL has an effect on the enhancement of the ferroelectric phase. In addition, the device with ZrO2 regulating layer exhibits a superior ON/OFF conductance ratio, endurance, and retention characteristics, demonstrating potential for application to memory. This work provides an effective way to improve the ferroelectricity in HfAlO films at low annealing temperatures.