High-precision geological and mineralogical characterization methods will guide the development and testing of several distinct hypothesis-driven extraction approaches for the nation’s largest lithium resource. This approach motivates thorough examination of lithium mudrock mineralogy and thermochemistry to inform novel methods of lithium separation. The major goals of the proposed work will follow from two simultaneous technical tasks. One is characterizing the nature of lithium (Li) and other critical materials from the McDermitt caldera deposit. The other is testing novel metallurgical extraction methods for Li from these resources.