Pegmatitic deposits of critical metals (e.g., Li, Ta, Be) are becoming increasingly significant, with growing interest in understanding metal enrichment processes and potential vectors to aid the discovery of new resources. In southeast Ireland, the Leinster pegmatite belt comprises several largely concealed Li-Cs-Ta albite-spodumene-type pegmatites. We carried out detailed mineralogical characterization and whole-rock geochemical analyses of six drill cores intersecting pegmatite bodies and their country rocks. Exomorphic halos 2–6 m thick, enriched in Li, Rb, Be, B, Cs, Sn and Ta, are identified in both mica schists and granitic rocks adjacent to spodumene pegmatites. Metasomatism in wall rocks visible to the naked eye is restricted to a few tens of centimeters, suggesting country rock permeability plays a key role in the dispersion of these fluids. We propose that halos result from the discharge of rare element-rich residual fluids exsolved near the end of pegmatite crystallization. Halo geochemistry reflects the internal evolution of the crystallizing pegmatite system, with residual fluid rich in incompatible elements accumulated by geochemical fractionation (Be, B, Cs, Sn, Ta) and by auto-metasomatic resorption of spodumene and K-feldspar (Li, Rb). The possibility of identifying rare-element enrichment trends by analysis of bedrock, stream sediments and soils brings opportunities for mineral exploration strategies in Ireland and for similar albite-spodumene pegmatites worldwide.