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Recent developments in inherently selective atomic layer deposition (ISALD) resulted in the deposition of amorphous ZrO₂thin 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) ZrO₂film. 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 ZrO₂film within minutes of exposure. Moreover, outward diffusion of the nucleated tetragonal ZrO₂away from the interface was also observed.