Formation of the giant Chicxulub crater off Mexico's Yucatan Peninsula coincided with deposition of the global Ir-rich Cretaceous-Tertiary (K-T) stratigraphic boundary layer at ca. 65 Ma. The boundary is marked most sharply by abundant spherules containing unaltered grains of magnesioferrite spinel. Here we predict for the first time the sequential condensation of solids and liquids from the plume of vaporized rock expected from oblique K-T impacts. We predict highly oxidizing plumes that condense silicate liquid droplets bearing spinel grains whose compositions closely match those marking the actual boundary. Systematic global variations in spinel composition are consistent with higher condensation temperatures for spinels found at Atlantic and European sites than for those in the Pacific.