Recent national assessments highlight U.S. reliance on imported rare-earth elements and advanced alloy feedstocks. Federal critical materials strategies emphasize the importance of developing alternative material platforms capable of maintaining performance while utilizing domestically accessible elements. A central motivation of this research is the development of high-entropy alloys and their nanostructures as next-generation materials platforms capable of reducing reliance on critical and supply-constrained materials. Many advanced structural, catalytic, and energy technologies depend heavily on materials containing titanium and rare-earth elements that are subject to geopolitical supply vulnerabilities and concentrated global production. Our research provides a transformative materials design strategy enabling the creation of high-performance alloys using more abundant and geographically diversified elements. This design strategy allows high entropy alloys to achieve mechanical strength, catalytic efficiency, and thermal stability comparable to or exceeding conventional critical-element-based materials while reducing supply chain vulnerabilities.