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Laser-induced breakdown spectroscopy (LIBS), which has recently emerged as tool for geochemical analysis outside the traditional laboratory setting, is an ideal tool for Li exploration because it is the only technique that can measure Li in minerals, rocks, soils, and brines in-situ in the field. In addition to being used in many products essential to modern life, Li is a necessary element for a reduced carbon future and Li–Cs–Ta (LCT) granitic pegmatites are an important source of Li. Such pegmatites can have varying degrees of enrichment in Li, Rb, Cs, Be, Sn, Ga, Ta>Nb, B, P, and F. We focus here on the LCT pegmatites of the Carolina Tin-Spodumene Belt (CTSB) situated in the Kings Mountain Shear Zone, which extends from South Carolina into North Carolina. The CTSB hosts both barren and fertile pegmatites, with Li-enriched pegmatites containing spodumene, K-feldspar, albite, quartz, muscovite, and beryl. We illustrate how handheld LIBS analysis can be used for real-time Li analysis in the field at a historically important CTSB pegmatite locality in Gaston County, N.C. in four contexts: (i) elemental detection and identification; (ii) microchemical mapping; (iii) depth profiling; and (iv) elemental quantitative analysis. Finally, as an example of a practical exploration application, we describe how handheld LIBS can be used to measure K/Rb ratios and Li contents of muscovite and rapidly determine the degree of pegmatite fractionation. This study demonstrates the potential of handheld LIBS to drastically reduce the time necessary to acquire geochemical data relevant to acquiring compositional information for pegmatites during a Li pegmatite exploration program. [ABSTRACT FROM AUTHOR]