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ZrTiOx-based metal-insulator-metal (MIM) devices with both-sided, one-sided, and without interfacial layer (IL) were fabricated by employing Ni or TaN as the electrodes to investigate the impact of presence and position of IL on the resistive switching behaviors. The IL plays a critical role in determining the magnitude of SET and RESET voltage since the oxygen vacancies and trapped electrons in the IL modulate the effective electric field in the ZrTiOx. With Ni and TaN as the top and bottom electrode, respectively, devices demonstrate self-compliance and bipolar switching behavior without requiring a forming step. The devices also exhibit great potential for next-generation nonvolatile memory applications because of the promising characteristics such as low dc SET/RESET voltage of 0.9/-0.6 V, tight distribution of device parameters, high switching speed of 200 ns with ±1.3 V, a large memory window of 6000 times, robust endurance up to 106 cycles, and good retention.