Between 1924 and 1947, Gino Severini decorated five churches in the Romand region of Switzerland with monumental religious wall paintings. This mural art played an important role in the Italian artist's career despite being mostly unknown and not easily found. The painting methods and materials of these modern Swiss murals were characterized by combining historical and archival research with onsite visual and scientific examination. Most pigments were identified with noninvasive methods integrating mapping techniques (i.e., technical photography and digital microscopy) with point analysis (x‐ray fluorescence and reflection FT‐IR spectroscopy). The results of these portable techniques were completed with SEM‐EDS, μFT‐IR FPA imaging, and μRaman analyses on micro‐samples which provided stratigraphic and compositional information to complement the noninvasive results. Overall, the data obtained show that Severini used both traditional pigments (e.g., Sangiovanni white and ochres/earths of various color) and modern ones, such as cadmium‐based pigments, with different painting techniques (e.g., zinc white was applied exclusively a secco). Apart from cerulean blue (cobalt stannate) and Naples yellow (lead antimonate) found only in two locations, the same set of pigments was documented in all of Severini's Swiss murals. The characterization of the artist's palette is important to understand the technical painting process followed by Severini, his interest on new painting materials available on the market and, at the same time, loyalty towards traditional painting methods, such as painting a fresco.