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This paper presents the findings of the first multi-analytical investigation of the Book of Uí Mhaine, one of the largest Gaelic Books surviving from the medieval vernacular period. A combination of protein analysis, point X-ray fluorescence spectroscopy (XRF), multispectral imaging (MSI), point Fiber-Optic Reflectance Spectroscopy (FORS) and point Raman spectroscopy was used to perform a systematic investigation of the Book of Uí Mhaine's constituent materials, including parchment, inks and pigments. The analysis revealed that the parchment was made of calfskin, both blunt tools and Pb-containing materials were used for ruling the pages throughout the manuscript, and iron-based inks were used to write the content of the book. The decoration was restricted to the initial letters and rubrication across the body text. The decoration color palette was limited to yellow and red, comprising arsenic-, mercury- and lead-based pigments. A copper-based green pigment was found only on one folio. The scientific knowledge acquired through this multi-analytical approach complemented a substantial corpus of knowledge already built by Gaelic scholars, paleographers, codicologists and conservators. This work not only allowed for the consolidation of existing information on methods and materials used for the production of medieval Gaelic manuscripts but also laid the basis for future comparative work with other contemporary traditions in Ireland and Europe. [ABSTRACT FROM AUTHOR]