This report presents the fabrication and pressure-driven processing of heterostructural nanocrystal superlattices (HNC-SLs) self-assembled from quantum-dot-Au (QD-Au) satellite-type HNCs. In situ small/wide-angle X-ray scattering and electron microscopic measurements showed that the HNC-SLs underwent structural transformation at both atomic- and mesoscales during the pressure processing. Upon deviatoric stress-driven orientational migration, the intraparticle coalescence of Au satellites at QD surfaces transforms individual HNCs into heterodimers, whereas the interparticle fusion drives assembled HNCs into ordered heterorod arrays. These results demonstrate high-pressure-processing as a clean and fast means for conversion of HNCs into novel heteromaterials that are difficult to achieve through conventional synthetic routes.