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Protein\u2010based strategies offer selective and sustainable alternatives to conventional separation processes. While native proteins have been identified for REE processing, protein engineering to enhance the separation of REE mixtures remains constrained by low\u2010throughput methods that limit the exploration of amino acids beyond the metal coordination sphere. Here, we developed a selection circuit based on a lanthanide\u2010mediated protein\u2010protein interaction for phage\u2010assisted continuous evolution (PACE). This system rapidly selected an evolving calmodulin\u2010derived peptide library, yielding a dominant sequence within days. Molecular dynamics simulations of the evolved protein suggest a restructured hydrogen\u2010bond network, which enhances second\u2010shell ion coordination and protein packing. These changes improved binding affinity and thermal stability, enabling single\u2010stage, chelator\u2010free, high\u2010purity separations of individual REEs. This high\u2010throughput approach can be readily extended to evolve other critical metal\u2010binding proteins.<\/jats:p>","DOI":"10.1002\/anie.202514785","type":"journal-article","created":{"date-parts":[[2026,2,5]],"date-time":"2026-02-05T06:08:56Z","timestamp":1770271736000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["Continuous Evolution of Calmodulin for High\u2010Purity Separation of Rare Earth Elements"],"prefix":"10.1002","volume":"65","author":[{"given":"Farid F.","family":"Khoury","sequence":"first","affiliation":[{"name":"Department of Chemical Engineering Columbia University  New York New York USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Sameera","family":"Abeyarthna","sequence":"additional","affiliation":[{"name":"Department of Chemical Engineering Columbia University  New York New York USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mallori 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