The chemistry of surviving pieces of Eoarchaean mantle together with related crust helps us determine early crust-forming mechanisms. Two lenses of high-Mg, low-Al dunite within a ca. 3720 Ma part of the Isua supracrustal belt in Greenland are interpreted as relicts of Eoarchaean mantle with minimal crustal disturbance. The lenses are within altered, higher Al, Ca ultramafic schists and are intercalated with amphibolitized pillow basalts and gabbros with island arc chemical signatures, all intruded by 3715–3710 Ma tonalites. One variety of dunite is dominated by forsterite (Fo90–92) olivine with accessory chromite and rare clinopyroxene, which does not show high field strength element (HFSE) anomalies. Another variety contains olivine (Fo96–98), some intergrown with Ti-humite group minerals with strong positive HFSE anomalies that are complementary to the negative HFSE anomalies of the adjacent amphibolites. We propose that these dunites are tectonic slivers of ca. 3720 Ma subarc mantle that preserve evidence for varying interaction with mafic magmas in a ≥850 °C, 1.7–2.0 GPa subcrustal environment. These are by far the oldest direct geochemical link between coeval mantle and crustal rocks, and are new evidence for subduction zone–like environments on the early Earth.