At a former uranium pilot mill in Grand Junction, Colorado, mine tailings and some subpile sediments were excavated to various depths to meet surface radiological standards, but residual solid-phase uranium below these excavation depths still occurs at concentrations above background. The combination of fission-track radiography and scanning electron microscope energy-dispersive X-ray spectroscopy (SEM-EDS) provides a uniquely efficient and quantitative way of determining mineralogic associations of uranium that can influence uranium mobility. After the creation of sample thin sections, a mica sheet is placed on those thin sections and irradiated in a nuclear research reactor. Decay of the irradiated uranium creates fission tracks that can be viewed with a microscope. The fission-track radiography images indicate thin section sample areas with elevated uranium that are focus areas for SEM-EDS work. EDS spectra provide quantitative elemental data that indicate the mineralogy of individual grains or grain coatings associated with the fission-track identification of elevated uranium. For the site in this study, the results indicated that uranium occurred (1) with coatings of aluminum–silicon (Al/Si) gel and gypsum, (2) dispersed in the unsaturated zone associated with evaporite-type salts, and (3) sorbed onto organic carbon. The Al/Si gel likely formed when low-pH waters were precipitated during calcite buffering, which in turn retained or precipitated trace amounts of Fe, As, U, V, Ca, and S. Understanding these mechanisms can help guide future laboratory and field-scale efforts in determining long-term uranium release rates to groundwater.