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In ultrashort-pulsed laser processing, surface modification is subject to complex laser and scanning parameter studies. In addition, quality assurance systems for monitoring surface modification are still lacking. Automated laser processing routines featuring machine learning (ML) can help overcome these limitations, but they are largely absent in the literature and still lack practical applications. This paper presents a new methodology for machine learning classification of self-organized surface structures based on light microscopic images. For this purpose, three application-relevant types of self-organized surface structures are fabricated using a 300 fs laser system on hot working tool steel and stainless-steel substrates. Optical images of the hot working tool steel substrates were used to learn a classification algorithm based on the open-source tool Teachable Machine from Google. The trained classification algorithm achieved very high accuracy in distinguishing the surface types for the hot working steel substrate learned on, as well as for surface structures on the stainless-steel substrate. In addition, the algorithm also achieved very high accuracy in classifying the images of a specific structure class captured at different optical magnifications. Thus, the methodology proposed represents a simple and robust automated classification of surface structures that can be used as a basis for further development of quality assurance systems, automated process parameter recommendation, and inline laser parameter control.