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Recent developments in inherently selective atomic layer deposition (ISALD) resulted in the deposition of amorphous ZrO2 thin film on Si with a high growth rate (2 Å/cycle). The deposited film with a high dielectric constant via ISALD may be used in semiconductor processing. However, the amorphous nature of the film and the ZrO2–SiO2/Si interface must be assessed to ensure the prevention of leakage current. There is little information available in the literature regarding the ZrO2–SiO2/Si interface of atomic layer deposition (ALD) ZrO2 film. In this study, high‐resolution transmission electron microscopy was extensively used to determine whether the film and the interface were crystalline or amorphous. It was interesting to find that a high‐energy electron beam can induce crystallinity in the amorphous as‐deposited ZrO2 film within minutes of exposure. Moreover, outward diffusion of the nucleated tetragonal ZrO2 away from the interface was also observed.