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Laser cleaning is a competitive alternative to ablate and remove the hard oxide layer on hot-rolled stainless steel. To meet the practical demand, laser-induced breakdown spectroscopy (LIBS) was applied for real-time monitoring of the cleaning process in this study. Furthermore, the as-received and laser cleaned surfaces were characterized by an optical micrograph, an X-ray diffractometer, and a laser scanning confocal microscope. The results showed the relative intensity ratio (RIR) of the Fe_I emission line at 520.9 nm and the Cr_I emission line at 589.2 could be a quantitative index to monitor the cleaning process. When the oxide layer was not fully cleaned, the LIBS signals of the substrate were not excited, and the ratio was almost invariant as the power of the laser increased. However, it sharply increased once the oxide layer was effectively cleaned, the cleaned surface was bright, and the surface roughness was smaller in this case. Subsequently, as the surface was over-cleaned with the further increase of laser power, the RIR value remained large. The optimal laser cleaning parameters obtained by the monitoring were determined to avoid re-oxidation and reduce the roughness of the cleaned surface.