Sanukitoids represent a volumetrically minor but important series of Neoarchean granitoids enriched in large-ion lithophile elements (e.g., Ba, Sr, and light rare earth elements), and with relatively high compatible elements (e.g., Mg, Ni, and Cr). Petrogenetic models have favored an origin in the suprasubduction mantle wedge, so their sudden appearance ca. 2.95–2.68 Ga has made them central to the ongoing debate about the beginnings of modern plate tectonics. Caledonian high Ba-Sr granites from the Northern Highlands of Scotland are petrological and compositional equivalents. The Caledonian examples have not undergone subsequent reworking, and their petrogenetic setting can be used to inform genetic models for sanukitoids. Prolonged subduction preceded emplacement of the high Ba-Sr granites in a short interval (∼10 Ma) at the end of the Caledonian orogeny. Sediment subduction was responsible for elemental and isotopic enrichments and slab breakoff triggered melting in the subcontinental lithospheric mantle. This implies that during the Neoarchean the evolving tectonothermal regime moved the locus of melting from the basaltic slab to the sediment-infused mantle wedge, creating the first subcontinental lithospheric mantle. Sanukitoids may then have resulted from widespread, closely subsequent slab-breakoff events, producing evolved magmas by familiar fractionation mechanisms. Careful study of secular variations in high Ba-Sr magmas could constrain the evolution of the subcontinental lithosphere.