Paleoarchean rocks of the tonalite–trondhjemite–granodiorite (TTG) series require a basaltic source region more enriched in K, LILE, Th and LREE than the low-K tholeiites typical of Archean supracrustal sequences. Most TTG of the Pilbara Craton, in northwestern Australia, formed between 3.5 and 3.42 Ga through infracrustal melting of a source older than 3.5 Ga. Basaltic to andesitic rocks of the 3.51 Ga Coucal Formation, at the base of the Pilbara Supergroup, are amongst the only well-preserved remnants of pre-3.5 Ga supracrustal material on Earth, and may have formed a large proportion of pre-3.5 Ga Pilbara crust. These rocks are significantly enriched in K, LILE, Th and LREE compared to post-3.5 Ga Paleoarchean basalts and andesites, and form a compositionally suitable source for TTG. Enrichment in these basalts was not the result of crustal assimilation but was inherited from a mantle source that was less depleted than modern MORB-source and was enriched in recycled crustal components. We suggest that the formation of Paleoarchean TTG and of their voluminous mafic source regions reflects both a primitive stage in the thermal and compositional evolution of the mantle and a significant prehistory of crustal recycling.