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This article reports an improvement in the performance of the hafnium oxide-based (HfO 2 ) ferroelectric field-effect transistors (FeFET) achieved by a synergistic approach of interfacial layer ( IL ) engineering and READ -voltage optimization. FeFET devices with silicon dioxide (SiO 2 ) and silicon oxynitride (SiON) as IL were fabricated and characterized. Although the FeFETs with SiO 2 interfaces demonstrated better low-frequency characteristics compared to the FeFETs with SiON interfaces, the latter demonstrated better WRITE endurance and retention. Finally, the neuromorphic simulation was conducted to evaluate the performance of FeFETs with SiO 2 and SiON IL as synaptic devices. We observed that the WRITE endurance in both types of FeFETs was insufficient to carry out online neural network training. Therefore, we consider an inference-only operation with offline neural network training. The system-level simulation reveals that the impact of systematic degradation via retention degradation is much more significant for inference-only operation than low-frequency noise. The neural network with FeFETs based on SiON IL in the synaptic core shows 96% accuracy for the inference operation on the handwritten digit from the Modified National Institute of Standards and Technology ( MNIST ) data set in the presence of flicker noise and retention degradation, which is only a 2.5% deviation from the software baseline., Competing Interests: The authors declare no competing financial interest., (© 2022 from Fraunhofer-Gesellschaft (CNT, Fraunhofer IPMS). Published by American Chemical Society.)