The mainland Lewisian Gneiss Complex (LGC) in NW Scotland is dominated by Archean tonalite-trondhjemite-granodiorite (TTG) gneisses. It consists of at least three distinct crustal blocks that have different magmatic and metamorphic histories. The LGC is regarded to either represent i) a once-contiguous fragment of Archean crust that was later disaggregated and reassembled along major shear zones into the northern, central and southern regions, or ii) a collage of discrete terranes. To better assess the tectono-magmatic evolution of the LGC, we use in situ U-Pb, Lu-Hf and trace element analysis of zircon grains derived from a representative set of TTG gneiss samples. The crystallization ages of TTGs range between 2778 and 2609 Ma in the northern region (Rhiconich terrane), 3003 and 2731 Ma in the central region (Assynt/Gruinard terranes), and 3110 and 2675 Ma in the southern region (Rona terrane). Zircon εHf(t) values of the oldest samples from the southern region are broadly chondritic. Samples from the southern part of the central region (Gruinard terrane) are more radiogenic, indicating a major period of juvenile magmatism at c. 2900-2800 Ma. Zircon derived from TTGs < 2800 Ma is characterised by chondritic to sub-chondritic Hf isotope signatures, pointing to increased crustal reworking during the late stages of TTG magmatism. Collectively, our data show that TTGs in the different parts of the LGC formed at different conditions and from different sources. We propose that the LGC is composed of at least three terranes that were assembled during the Neoarchean to Paleoproterozoic.