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Here, we introduce a cyclodextrin\u2010regulated interfacial microenvironment that delivers a Faradaic efficiency (FE) of up to 88% for pyrazine hydrogenation at \u2212100\u00a0mA\u00a0cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    . The hydroxyl\u2010rich outer surface disrupts the ordered hydrogen\u2010bond network by inhibiting the reorientation of interfacial H\n                    <jats:sub>2<\/jats:sub>\n                    O, facilitating the migration of the reactant to the electrode surface. Simultaneously, the hydrophobic cavities selectively recognize and bind substrates via host\u2013guest interactions, creating oriented shuttle channel that lowers the transfer energy barrier and accelerates mass transport kinetics. This strategy can be extended to diverse hydrogenation reactions and to other deuteration reactions with improved FE at \u2212100\u00a0mA\u00a0cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    . Moreover, the synthesis of deuterated piperazines and their conversion into deuterium\u2010labeled drugs highlights their practical potential. This work provides a general interfacial engineering strategy to overcome mass transport bottlenecks in electrosynthesis, with broad implications for the production of high\u2010value chemicals and isotopically labeled compounds.\n                  <\/jats:p>","DOI":"10.1002\/anie.9228845","type":"journal-article","created":{"date-parts":[[2026,9,7]],"date-time":"2026-09-07T12:57:11Z","timestamp":1788785831000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Host\u2013Guest Chemistry Creates an Oriented Shuttle Channel to Overcome Mass Transport Limitations in Electrocatalytic Hydrogenation"],"prefix":"10.1002","author":[{"given":"Yunjia","family":"Liu","sequence":"first","affiliation":[{"name":"Institute of Molecular Plus Department of Chemistry School of Science Tianjin University  Tianjin 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