Mantle lithologies in orogenic massifs and xenoliths commonly display strikingly different Hf- and Nd-isotope compositions compared to oceanic basalts. While the presence of pyroxenites has long been suggested in the source region of mantle-derived magmas, very few studies have reported their combined HfNd isotope compositions. We here report the first LuHf data along with ReOs data and S concentrations on the Cabo Ortegal Complex, where the pyroxenite-rich Herbeira massif has been interpreted as remnants of a delaminated arc root. The pyroxenites, chromitites and their host harzburgites show a wide range of whole-rock 187Re/188Os and 187Os/188Os (0.16–1.44), indicating that Re was strongly mobilized, partly during hydrous retrograde metamorphism but mostly during supergene alteration that preferentially affected low-Mg#, low Cu/S pyroxenites. Samples that escaped this disturbance yield an isochron age of 838 ± 42 Ma, interpreted as the formation of Cabo Ortegal pyroxenites. Corresponding values of initial 187Os/188Os (0.111–0.117) are relatively unradiogenic, suggesting limited contributions of slab-derived Os to primitive arc melts such as those parental to these pyroxenites. This interpretation is consistent with radiogenic Os in arc lavas being mostly related to crustal assimilation. Paleoproterozoic to Archean Os model ages confirm that Cabo Ortegal pyroxenites record incipient volcanic arc magmatism on the continental margin of the Western African Craton, as notably documented by zircon UPb ages of 2.1 and 2.7 Ga. LuHf data collected on clinopyroxene and amphibole separates and whole-rock samples are characterized by uncorrelated 176Lu/177Hf and 176Hf/177Hf (0.2822–0.2855), decoupled from Nd-isotope compositions. This decoupling is ascribed to diffusional disequilibrium during melt-peridotite interaction, in good agreement with the results of percolation-diffusion models simulating the interaction of an arc melt with an ancient melt-depleted residue. These models notably show that HfNd isotopic decoupling such as recorded by Cabo Ortegal pyroxenites and peridotites (ΔƐHf(i) up to +97) is enhanced during melt-peridotite interaction by slow diffusional re-equilibration and can be relatively insensitive to chromatographic fractionation. Finally, we discuss the hypothesis that arc-continent interaction may provide preferential conditions for such isotopic decoupling and propose that its ubiquitous recognition in peridotites reflects the recycling of sub-arc mantle domains derived from ancient, reworked SCLM.