Rare earth materials play an irreplaceable role in biomedical and high technology fields. However, typical mining and extraction approaches to rare earth elements (REEs) often lead to severe environmental problems and resource wastage due to the involvement of hazardous chemicals. Although biomining shows elegant alternatives, there are still grand challenges to sustainably isolate and recover REEs in nature because of insufficient metal‐extracting microbes and RE‐scavenging macromolecular tools. To obtain high‐performance rare earth materials directly from rare earth ore, a new generation of biological synthesis strategies needs to be developed for the efficient preparation of REEs. The microbial synthesis system established here has achieved active biomanufacturing of high‐purity rare earth products. Further, through employing robust affinity columns bioconjugated with structurally engineered proteins, outstanding separation of Eu/Lu and Dy/La is acquired with the purity of 99.9% (Eu), 97.1% (La), and 92.7% (Dy). More importantly, in situ one‐pot synthesis of lanthanide‐dependent methanol dehydrogenase is well harnessed and exclusively adsorbs La, Ce, Pr, and Nd in RE tailing for advanced biocatalysis, indicating high value‐added application. Therefore, this novel biosynthetic platform provides an insightful roadmap to expand the scope of chassis engineering in terms of biofoundry and to manufacture valuable bioproducts related to REEs.