Lithium (Li) is one of the latest metals to be added to the list of critical materials in Europe and, thus, lithium exploration in Europe has become a necessity to guarantee its mid- to long-term stable supply. Laser-induced breakdown spectroscopy (LIBS) is a powerful analysis technique that allows for simultaneous multi-elemental analysis with an excellent coverage of light elements (Z < 13). This data paper provides more than 4000 LIBS spectra obtained using a handheld LIBS tool on approximately 140 Li-content materials (minerals, powder pellets, and rocks) and their Li concentrations. The high resolution of the spectrometers combined with the low detection limits for light elements make the LIBS technique a powerful option to detect Li and trace elements of first interest, such as Be, Cs, F, and Rb. The LIBS spectra dataset combined with the Li content dataset can be used to obtain quantitative estimation of Li in Li-rich matrices. This paper can be utilized as technical and spectroscopic support for Li detection in the field using a portable LIBS instrument.

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