The Central Mineral Belt (CMB) in Labrador, Canada, hosts multiple U (±base ± precious metal) showings, prospects and deposits in metamorphosed and variably hydrothermally altered Neoarchean to Mesoproterozoic, igneous and sedimentary rocks. Previous work has recognized U mineralization locally associated with Fe-Ca and alkali metasomatism typical of metasomatic iron oxide and alkali-calcic alteration systems (IOAA) that host iron oxide-copper-gold (IOCG) and affiliated critical metal deposits. However, the type, extent and temporal or genetic relationships between the diverse Fe, Ca and alkali metasomatism and the regionally distributed U mineralization remains poorly understood.Combined unsupervised machine-learning and classification of alteration from a large geochemical dataset distinguish the main alteration phases in the CMB, identify compositional changes related to U mineralization, and infer lithological/mineralogical information from samples with censored (i.e., missing), limited and/or inaccurate metadata. Weak to intense Na and Na + Ca-Fe (Mg) metasomatism in the southwest (Two-Time and Moran Lake areas) and eastern (Michelin area) portions of the CMB pre-dates U mineralization and Fe-oxide breccia development, similar to albitite-hosted U and IOCG deposits globally.Rare earth elements and spider diagrams highlight both preservation and disruption of normally immobile elements. Principal component and cluster analysis indicate significant variations in Fe-Mg ± Na contents in the rocks from combinations of Na, Ca, Fe, and Mg-rich alteration, while protolith REE signatures can be locally preserved even after pervasive albitization-hematization. Cluster analysis identifies mineralized felsic and mafic rocks in the Michelin deposit and Moran Lake area, facilitating inference of relevant lithological/mineralogical information from samples lacking or with limited meta-data.The methods outlined provide rapid and relatively inexpensive means to optimize identification of mineral systems within large geochemical datasets, verify drill core or field observations, highlight potentially overlooked alteration, and refine economic mineral potential assessments. Based on our results and previous work, we suggest the mineral potential of the southwestern and eastern CMB needs to be re-assessed with modern exploration models for IOAA ore systems and their iron oxide-poor variants.