Critical minerals (CMs) are pivotal in modern industries, such as telecommunications, defense, medicine, and aerospace, contributing significantly to regional and global economic growth. However, the reliance on external sources for 26 out of 50 identified CMs raises concerns about supply chain vulnerabilities. To address this, the research focused on developing a hydrometallurgical process for extracting cobalt, manganese, and nickel from acid mine drainage (AMD) treatment by-products, emphasizing the need to diversify CM supply chains within the United States (US). A solution composed of an REE solvent extraction raffinate loaded with cobalt, manganese, nickel, and various impurity metals was utilized as a feedstock in this study. The developed hydrometallurgical process involved initial sodium hydroxide precipitation to remove impurities like aluminum and iron from an SX raffinate solution generated during the extraction of rare earth elements (REEs). Precipitation stages were performed in a pH region ranging from 2 to 12 to identify the optimum pH values, achieving a tradeoff between recovery and impurity removal. A subsequent precipitation process at pH 5–10 yielded a product rich in CMs, such as manganese, cobalt, and nickel. Further separation steps involved nitric acid washing, resulting in a Mn product with a purity of 47.9% by weight and a solution with extractable concentrations of cobalt and nickel. Stagewise precipitation with sodium sulfide subsequently produced three solid products: cobalt and nickel product at pH 1–5, manganese product at pH 5–10, and magnesium at pH 10–12. The study also explored other separation approaches, including solvent extraction, to enhance the separation of nickel from cobalt. Overall, the developed hydrometallurgical process generated the following products with varying degrees of purities: cobalt (9.92 wt.%), nickel (14 wt.%), manganese (47.9 wt.%), and magnesium (27.49 wt.%). This research aimed to contribute to the sustainable extraction of CMs from secondary sources, reducing the US’ reliance on imports and promoting a more resilient supply chain for these crucial elements.