Many rare metals used today are derived from granitic pegmatites, but debate continues about the origin of these rocks. It is clear that some pegmatites represent the most highly fractionated products of a parental granite body, whilst others have formed by anatexis of local crust. However, the importance of these two processes in the formation of rare-metal pegmatites is not always evident.\ud \ud The Lewisian Gneiss Complex of NW Scotland comprises Archaean meta-igneous gneisses which were highly reworked during accretional and collisional events in the Palaeoproterozoic (Laxfordian orogeny). Crustal thickening and subsequent decompression led to melting and the formation of abundant granitic and pegmatitic sheets in many parts of the Lewisian Gneiss Complex. This paper presents new petrological, geochemical and age data for those pegmatites and shows that, whilst the majority are barren biotite-magnetite granitic pegmatites, a few muscovite-garnet (rare-metal) pegmatites are present. These are mainly intruded into a belt of Palaeoproterozoic metasedimentary and meta-igneous rocks known as the Harris Granulite Belt.\ud \ud The rare-metal pegmatites are distinct in their mineralogy, containing garnet and muscovite, with local tourmaline and a range of accessory minerals including columbite and tantalite. In contrast, the biotite-magnetite pegmatites have biotite and magnetite as their main mafic components. The rare-metal pegmatites are also distinguished by their bulk-rock and mineral chemistry, including a more peraluminous character and enrichments in Rb, Li, Cs, Be, Nb and Ta. New U-Pb ages (c. 1690–1710 Ma) suggest that these rare-metal pegmatites are within the age range of nearby biotite-magnetite pegmatites, indicating that similar genetic processes could have been responsible for their formation.\ud \ud The peraluminous nature of the rare-metal pegmatites strongly points towards a metasedimentary source. Notably, within the Lewisian Gneiss Complex, such pegmatites are only found in areas where a metasedimentary source is available. The evidence thus points towards all the Laxfordian pegmatites being formed by a process of crustal anatexis, with the formation of rare-metal pegmatites being largely controlled by source composition rather than solely by genetic process. This is in keeping with previous studies that have also challenged the widely accepted model that all rare-metal pegmatites are formed by fractionation from a parental granite, and raises questions about the origin of other mineralised pegmatites worldwide.\u