The Austroalpine Unit Pegmatite Province (AUPP) in the eastern European Alps hosts abundant Permian-aged, variably rare-metal-enriched pegmatite bodies. However, only a small number containing spodumene [LiAlSi2O6] have been discovered. Here, we characterize three drill cores from the AUPP’s largest spodumene pegmatite resource, the Wolfsberg deposit (Austria), to determine the extent of rare-metal halo formation within different host rock types generated by pegmatite-derived fluids and their applicability to spodumene pegmatite exploration. The halos in both mica schist and amphibolite host rocks, as quantified via whole-rock mass-balance calculations, are characterized by enrichments in Li, Cs, Sn, Rb and Tl, amongst others, elements which were highly mobile during initial interactions between pegmatite-derived fluids and host rocks. The concentrations of these elements within the halos can be several times that present in unaltered host rock. They are most enriched in altered host rock interbedded or at the contacts with pegmatite, and decrease with distance from pegmatite to a distance of at least 4 m in mica schist and <3 m in amphibolite. Lithium, and in mica schist, Cs, have the most consistent and furthest extending halos, with respective concentrations of >590 ppm and >40 ppm in mica schist, and >390 ppm Li in amphibolite indicating proximity to spodumene pegmatite. An ID-TIMS U-Pb titanite age of ca. 103 Ma derived from a rare-metal-enriched amphibolite within the alteration halo reflects recrystallization of the Permian protolith during the Cretaceous Alpine orogeny and indicates preservation of the original pegmatite signature through eclogite-facies metamorphism. Recognition of rare-metal halos surrounding pegmatite at Wolfsberg serves as a potential geochemical exploration tool for spodumene pegmatite within the AUPP and may be applicable to other regions.