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Recent work indicates that materials with nanoscale architectures, such as nanolayered Cu-Nb composites and nanoscale oxide dispersion-strengthened steels, are both thermally stable and offer improved performance under irradiation. Current understanding of the atomic-level response of such materials to radiation yields insights into how controlling composition, morphology, and interface-defect interactions may further enable atomic-scale design of radiation-tolerant nanostructured composite materials. With greater understanding of irradiation-assisted degradation mechanisms, this bottom-up design approach may pave the way for creating the extreme environment—tolerant structural materials needed to meet the world’s clean energy demand by expanding use of advanced fission and future fusion power.