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X-ray fluorescence (XRF) is a successful technique often used for the elemental analysis of cultural heritage artefacts. It is non-invasive, the equipment can be miniaturized and made portable and it allows addressing crucial issues such as the fabrication technology, authenticity and provenance of the artefacts. Depending on the components’ selection (e.g., the primary source, the detector and the focusing optics, if present), the analytical performance and the consequent suitability to investigate a given class of materials may vary significantly. The present paper discusses the analytical performance—with special regard to the limits of detection and the quantification uncertainty—of two portable XRF spectrometers developed within a collaboration between INFN-LNF-FISMEL and CNR-ISPC. The devices are expressly designed for heritage materials. In particular, one is equipped with focusing optics and it is intended to analyze small details on glasses and pigmented surfaces, whereas the other has a 70 kV X-ray tube, which greatly improves sensitivity for medium-Z elements, which is important in copper-based artefacts. Finally, this paper discusses two case studies to highlight the features of the instruments: one concerns Etruscan vitreous material beads and the other pre- and proto-historic copper-based artefacts from Tyrrhenian Central Italy. Thanks to the small size of the equipment, both investigations could easily be carried out in situ, namely, at the Museo Nazionale Etrusco in Rome and the Museo della Preistoria della Tuscia e della Rocca Farnese at Valentano.