In recent years, two end-member models for the formation of supercontinents have emerged. In the classical Wilson cycle, oceanic crust generated during supercontinent breakup (the interior ocean) is consumed during subsequent amalgamation so that the supercontinent turns “inside in” (introversion). Alternatively, following supercontinent breakup, the exterior margins of the dispersing continental fragments collide during reassembly so that the supercontinent turns “outside in” (extroversion). These end-member models can be distinguished by comparing the Sm-Nd crust-formation ages of accreted mafic complexes (e.g., ophiolites) in the collisional orogens formed during supercontinent assembly with the breakup age of the previous supercontinent. For supercontinents generated by introversion, these crust-formation ages postdate rifting of the previous supercontinent. For supercontinents generated by extroversion, the oceanic lithosphere consumed during reassembly predates breakup of the previous supercontinent, so that crust-formation ages of accreted mafic complexes are older than the age of rifting. In the Paleozoic Appalachian-Caledonide-Variscan orogen, a key collisional orogen in the assembly of Pangea, crust-formation ages of accretionary mafic complexes postdate the formation of the Iapetus Ocean (i.e., are younger than ca. 0.6 Ga), suggesting supercontinent reassembly by introversion. By contrast, the Neoproterozoic East African and Brasiliano orogens, which formed during the amalgamation of Gondwana, are characterized by mafic complexes with crust-formation ages (ca. 0.75–1.2 Ga) that predate the ca. 750 Ma breakup of Rodinia. Hence, these complexes must have formed from lithosphere in the exterior ocean that surrounded Rodinia, implying that this ocean was consumed during the amalgamation of Gondwana. These data indicate that Pangea and Gondwana were formed by introversion and extroversion, respectively, implying that supercontinents can be assembled by fundamentally distinct geodynamic processes.