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AbstractThis article is based on the MRS Medal presentation given by Delia J. Milliron at the 2023 MRS Fall Meeting & Exhibit in Boston, Mass. Milliron is cited “for the development of optically tunable metal oxide nanomaterials for applications such as energy-saving electrochromic windows.”Doped metal oxide nanocrystals (NCs) provide a highly tunable platform for localized surface plasmon resonance (LSPR) in the near- to mid-IR. This tunability can be achieved synthetically, through the size, shape, and composition of the NCs, or post-synthetically through reversible redox reactions, enabling a host of emerging applications. While the broad strokes of this tunability have been understood for a decade, over the last few years, there has been tremendous progress in understanding the relationships between the electronic structure, defect chemistry, and synthetic and post-synthetic tunability of metal oxide NCs. This article aims to provide an up-to-date picture of the optical tunability of metal oxide NC LSPR, in particular focusing on recent insights into how the NC electronic structure plays a role in LSPR tunability. Graphical abstract