The arrangement of atoms comprising a material determines its properties. Thus, atom arrangement controllability can substantially facilitate the creation of new materials such as functional materials. Relevant materials science research has relied heavily on heat treatments. This study investigates the phenomenon of atom rearrangement by applying a high‐frequency alternating current without heating. The proposed method spontaneously rearranges atoms to produce a dense crystal plane oriented parallel to the electron flow. The atoms are “shaken” by generating mechanical interaction between electrons and atoms. Transmission electron microscopy reveals the enlarged crystal grains and an increase in close‐packed planes resulting from the self‐alignment of the atoms along the direction of electron flow. Conventional heat treatments cannot result in such phenomena because heat treatments induce random vibration of the atoms. In contrast, the current flow in the high‐frequency alternating current enables direction‐specific vibration of the atoms. This novel technique could be applied to develop new functional materials that are difficult to obtain via conventional heat treatment methods. Furthermore, this atom rearrangement technology can be applied to expand the field of materials science research.

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