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This study introduces a Ta 2 O 5 -based self-rectifying memristor (SRM) with an Al 2 O 3 interfacial layer adopted to improve switching uniformity, read voltage margin, and long-term retention. The Pt/Ta 2 O 5 /Al 2 O 3 /TiN (PTAT) device exhibits a 10 5 rectification ratio, 10 4 on/off ratio, 2 × 10 6 endurance, and retention of 10 4 s at 150 °C. A 3-layer 4 × 4 vertical resistive random access memory structure exhibits uniform switching parameters. The coefficient of variation (CV) for device-to-device measurements is 0.23 for the low resistance state (LRS) and 0.22 for the high resistance state (HRS), while for cycle-to-cycle measurements, the CV is 0.38 for the LRS and 0.11 for the HRS. Finally, the present study demonstrates the superior performance of the PTAT devices in the context of hardware-aware training for a fully connected neural network implementation. These advancements position the PTAT device as a promising candidate for high-density three-dimensional storage class memory and low-power neural networks, offering the consistent performance and reliability necessary for future high-density storage applications.