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Mat-Eater with Pennants, a rarely exhibited sculpture in Alexander Calder’s oeuvre, was commissioned by The Museum of Modern Art (MoMA) and installed in 1945. To exhibit the large standing mobile in Alexander Calder: Modern from the Start (2021), the derelict sculpture had to be remediated; this initiated a collaborative investigation with conservation scientists, conservators, curators, and the Calder Foundation into the original paint colors hidden beneath layers of repaint. XRF analysis was carried out to elucidate the paints’ composition, followed by sampling for analysis to assess the paint stratigraphy and binders. Scrapings were analyzed by µ-FTIR and Raman spectroscopies; cross sections were examined with optical microscopy and analyzed with SEM-EDS. Analysis differentiated between the original paints, which contain Prussian blue, parachlor red, chrome yellow, and the many layers of overpaint, which contain titanium white, molybdate orange, a variety of β-Naphthol reds, red lead, and ultramarine. A model for Man-Eater, Mobile with 14 Flags, is also part of the museum’s collection, and was first considered as a point of reference for the original colors. Similar analysis, however, indicates that the maquette was painted after the Man-Eater was first installed, therefore is not representative of the original colors. In addition to investigating an early primary palette for Calder’s outdoor sculptures, this study helped develop the plan for the restoration of the original color scheme of Man-Eater.