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A compilation of mineral and glass compositions erupted at Villarrica volcano, Chile, measured by electron microprobe. Data are sourced from published articles, theses and unpublished works. Minerals and glasses are from deposits erupted over the last 100ka. This is supporting data for the manuscript entitled 'Insights into Magma Storage Beneath a Frequently Erupting Arc Volcano (Villarrica, Chile) from Unsupervised Machine Learning Analysis of Mineral Compositions' by F. O. Boschetty, D. J. Ferguson, J. A Cortés, E. Morgado, S. K. Ebmeier, D. J. Morgan, J. E. Romero and C. Silva Parejas.