Secondary ionization mass spectrometry (SIMS) U/Pb dating of zircon has been applied to rocks of the Lewisian Complex of South Harris (Outer Hebrides, NW Scotland), yielding insights into the complex geological evolution of this region and enhancing our understanding of terranes in the Lewisian Gneiss Complex. Results show that tonalite–trondhjemite–granodiorite magmatism occurred in the Tarbert Terrane between c. 2850 and 2830 Ma, equivalent to similar rocks in other parts of the Outer Hebrides. Magmatism was accompanied or closely followed by high-grade metamorphism at c. 2830 Ma, the first reported occurrence of such an event at this time. These rocks were affected by a subsequent high-grade metamorphic event at c. 2730 Ma, which has correlatives both in the Outer Hebrides and in the mainland Lewisian Gruinard Terrane. These data suggest that the ‘terranes’ forming the Outer Hebrides and parts of the mainland Lewisian were once contiguous and were fragmented by post-2730 Ma events. The c. 1700–1660 Ma ages from felsic sheets and pegmatites within the Langavat Shear Zone may record the reassembly of these crustal fragments.