Abstract: Highly efficient controlling the individual atomic migration is the basis of the modern atomic manufacturing. Although one-by-one atom migration can be realized precisely by STM technique, such a delicate operation is time consuming and restrictive conditions (e.g., high-vacuum) needed to be satisfied. Here, we reported that individual metal atoms can be efficiently transferred from the nanoparticle surface to the underneath substrate via instantaneous laser irradiation under ambient conditions. By inserting self-assembled monolayer (SAM) molecules into nanoparticle-on-mirror (NPoM) structures, a pronounced resonance shift that depends on the dipole moments of the SAM molecules, was observed upon laser irradiation. Assisted by the in-situ measurement of Raman spectra, synchronously capturing dark-field (DF) scattering spectra and DF imaging, it is clarified that the laser-induced localized surface plasmons, which generates strong dipole–dipole interactions, play a critical role in triggering atomic migration. Our study opens an avenue for the highly efficient fabrication of atomic patterns.