Surface patterning in the micro- and nanometer-range by means of pulsed laser interference has repeatedly proven to be a versatile tool for surface functionalization. With these techniques, however, the surface is often changed not only in terms of morphology but also in terms of surface chemistry. In this study, we present an in-depth investigation of the chemical surface modification occurring during surface patterning of copper by ultrashort pulsed direct laser interference patterning (USP-DLIP). A multimethod approach of parallel analysis using visualizing, topography-sensitive, and spectroscopic techniques allowed a detailed quantification of surface morphology as well as composition and distribution of surface chemistry related to both processing and atmospheric aging. The investigations revealed a heterogeneous surface composition separated in peak and valley regions predominantly consisting of Cu2O, as well as superficial agglomerations of CuO and carbon species. The evaluation was supported by a modeling approach for the quantification of XPS results in relation to heterogeneous surface composition, which was observed by means of a combination of different spectroscopic techniques. The overall results provide a detailed understanding of the chemical and topographical surface modification during USP-DLIP, which allows a more targeted use of this technology for surface functionalization.