This article describes the first results of a study of the collection of art materials, painted works, and techniques, belonging to the Lasar Segall Museum in Brazil, using materials and documents of the early 20th century. The paint materials from the museum's collection consist of over a hundred glass vases, tubes, and packets containing powdered pigments, inks, oils, and varnishes.Powdered and dried ink (labeled "ink for posters") samples were analyzed using confocal Raman microscopy spectroscopy, Fourier transform infrared spectroscopy, energy-dispersive X-ray fluorescence, and X-ray diffraction. The artist's palette chromophores such as ultramarine, cobalt and Prussian blue, goethite, hematite, and magnetite from natural ochres, lead basic carbonate, lead carbonate, anatase, zinc carbonate hydroxide, zinc oxide, lead chromate, carbon, cadmium sulfide, copper acetate arsenite, verditer, celadonite, serrabrancaite, vermilion, PY1, PY3, PR3, and PO5 were identified mainly by Raman spectroscopy. The color palette found in paintings from 1919 is closely related to the characterized pigments from the museum. Nevertheless, the violets found are not mineral in nature but organic. The descriptions of the results for each sample and painting were made available to the museum to assist in future conservation, dating, and authentication procedures of the works.