Abstract: Geochemical and geochronologic data are presented for meta-mafic to meta-felsic rocks along the Paleo-Tethys Suture in the Binalood Mountains east of Neyshabur, NE Iran. The rocks have a late Cambrian age (U–Pb zircon, ~ 490 Ma) and were metamorphosed in the Early Jurassic (40Ar/39Ar amphibole and plagioclase, 199–192 Ma). The rocks of this suite are alkaline and sub-alkaline (tholeiitic). The alkaline rocks are enriched in light relative to heavy rare earth elements, and do not show depletion of high-field strength elements on primitive mantle-normalized multi-element diagrams; they are similar to ocean island basalts (OIB). The tholeiitic rocks are depleted in Nb and Ta and have higher MgO and lower TiO2 than the alkaline rocks. Both types have similar, high and variable 87Sr/86Sr(i) isotopic compositions of 0.7044 to 0.7082 and 143Nd/144Nd(i) values of 0.5118 to 0.5122. The alkaline rocks are lower-degree partial melts than the tholeiitic rocks and were generated at greater depths; they likely originated from a garnet pyroxenite-rich source. The spatial, temporal, and geochemical relationships of early Paleozoic meta-mafic to felsic rocks along the Paleo-Tethys Suture (e.g., Shahrud, Jajarm, Binalood, Torbat-e-Jam) substantiate the role of a mantle plume in continental breakup along the northern margin of Gondwana and a late Cambrian-Ordovician onset of rifting that resulted in the opening of the Paleo-Tethys Ocean. The Early Jurassic metamorphism post-dates its closure. Graphical abstract: [Figure not available: see fulltext.].