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This work presents a dual spatial confinement strategy to synthesize uniformly dispersed, sub\u2010nanometer RuBi bimetallic hetero\u2010clusters embedded within porous carbon nanofibers (RuBi HCs\/PCNFs). The synthetic approach utilizes the internal pores of metal\u2010organic frameworks as primary nano\u2010reactors, coupled with an electrospun polymer matrix as a secondary physical barrier, preventing metal migration and coalescence during high\u2010temperature pyrolysis. We employ the alkaline hydrogen evolution reaction (HER) as a probe to evaluate the efficacy of this structural design. Characterizations and theoretical analysis show that the atomic proximity and electronic interactions between Ru and Bi optimize intermediate adsorption and accelerate the rate\u2010determining water dissociation step. Benefiting from these structural and electronic advantages, the RuBi HCs\/PCNFs catalyst delivers enhanced electrocatalytic HER activity and robust operational durability. When evaluated in an anion exchange membrane (AEM) water electrolyzer, the catalyst demonstrates stable, long\u2010term operation, showcasing the practical utility of the hetero\u2010cluster configuration. This study demonstrates the feasibility of utilizing dual spatial confinement to construct stable, sub\u2010nanometer bimetallic platforms for electrocatalytic applications.<\/jats:p>","DOI":"10.1002\/anie.2036983","type":"journal-article","created":{"date-parts":[[2026,10,8]],"date-time":"2026-10-08T05:59:31Z","timestamp":1791439171000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Highly Stabilized and Accessible Sub\u2010Nanometer RuBi Heteroclusters Drive Efficient Alkaline Hydrogen Evolution"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0004-1071-3925","authenticated-orcid":false,"given":"Qian","family":"Huang","sequence":"first","affiliation":[{"name":"College of Chemistry and Environmental Engineering Shenzhen University  Shenzhen Guangdong 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