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Phosphine oxides with different substituents are treated to prove the universality of this method. Computational approaches are applied to confirm that the reaction generated a C\u2550P double bond during the process, and the two\u2010electron reductive elimination process occurs with the assistance of the butadienyl backbone. The orbital interactions of the key transition states are clarified by principal interacting orbital (PIO) analysis. This work significantly expands the applicability of rare\u2010earth metallacycles and further reveals their unique reactivity, providing a C\u2500P coupling, azametallacycle, metallacycle, rare\u2010earth metal novel strategy for constructing phosphorus\u2010containing compounds.<\/jats:p>","DOI":"10.1002\/chem.202503142","type":"journal-article","created":{"date-parts":[[2025,12,31]],"date-time":"2025-12-31T13:57:59Z","timestamp":1767189479000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Carbon\u2010Phosphorus Cross\u2010Anion Coupling on Rare\u2010Earth Center"],"prefix":"10.1002","volume":"32","author":[{"ORCID":"https:\/\/orcid.org\/0009-0006-4963-2510","authenticated-orcid":false,"given":"Jinxiao","family":"Yang","sequence":"first","affiliation":[{"name":"Beijing National Laboratory For Molecular Sciences (BNLMS) State Key Laboratory of Rare Earth Materials Chemistry and Applications &amp; Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of Education Peking University  Beijing P.R. 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