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Abstract The emergence of memristive behavior in amorphous–crystalline 2D oxide heterostructures, which are synthesized by atomic layer deposition (ALD) of a few‐nanometer amorphous Al₂O₃layers onto atomically thin single‐crystalline ZnO nanosheets, is demonstrated. The conduction mechanism is identified based on classic oxygen vacancy conductive channels. ZnO nanosheets provide a 2D host for oxygen vacancies, while the amorphous Al₂O₃facilitates the generation and stabilization of the oxygen vacancies. The conduction mechanism in the high‐resistance state follows Poole–Frenkel emission, and in the the low‐resistance state is fitted by the Mott–Gurney law. From the slope of the fitting curve, the mobility in the low‐resistance state is estimated to be ≈2400 cm²V⁻¹s⁻¹, which is the highest value reported in semiconductor oxides. When annealed at high temperature to eliminate oxygen vacancies, Al is doped into the ZnO nanosheet, and the memristive behavior disappears, further confirming the oxygen vacancies as being responsible for the memristive behavior. The 2D heterointerface offers opportunities for new design of high‐performance memristor devices.