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Till date, there have been no direct atomic-level experimental observations of the earliest stages of the nucleation and growth processes of nanocrystals formed by thermally induced crystallization in ultrathin metallic glasses (MGs). Here, we present a study of the crystallization process in atomically thin and highly stable MG films using double spherical aberration-corrected scanning transmission electron microscopy (Cs-TEM). Taking advantage of the stability of MG films with a slow crystallization process and the atomic-level high resolution of Cs-TEM, we observe the formation of the nucleus precursor of nanocrystals formed by atom aggregation followed by concomitant coalescence and stepwise evolution of the shape of the nanocrystals with a monodispersed and separated bimodal size distribution. Molecular dynamics simulation of the atomic motion in the glass film on a rigid amorphous substrate confirms the stepwise evolution processes of atom aggregation, cluster formation, cluster movement on the substrate, and cluster coalescence into larger crystalline particles. Our results might provide a better fundamental understanding of the nucleation and growth processes of nanocrystals in thin MG films. [ABSTRACT FROM AUTHOR]