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However, the kinetic mismatch between key intermediates remains the major challenge for achieving selective C\u2012N coupling. Herein, indium\u2010doped titanium dioxide (In\u2010TiO\n                    <jats:sub>2<\/jats:sub>\n                    ) nanofibers were developed to regulate the hydrogenation pathway for realizing kinetics\u2010matched urea electrosynthesis. In situ spectroscopic analysis and theoretical calculations reveal that In doping reverses the hydrogenation pathway of nitrogen\u2010containing intermediates from the Eley\u2010Rideal (E\u2010R) to the Langmuir\u2013Hinshelwood (L\u2013H) mechanism. This shift is attributed to the sufficient *H supply guaranteed by the regulated interfacial water structure. Such reversed hydrogenation pathway balances *H utilization between CO\n                    <jats:sub>2<\/jats:sub>\n                    and NO\n                    <jats:sub>3<\/jats:sub>\n                    <jats:sup>\u2212<\/jats:sup>\n                    reduction, enabling well\u2010matched formation kinetics of key intermediates for efficient C\u2012N coupling. Owing to the above merits, In\u2010TiO\n                    <jats:sub>2<\/jats:sub>\n                    achieved the remarkable average urea yield rate of 56.5\u00a0mmol h\n                    <jats:sup>\u22121<\/jats:sup>\n                    g\n                    <jats:sup>\u22121<\/jats:sup>\n                    with a Faradaic efficiency of 32.8%. This work provides mechanistic insights into the hydrogenation pathways regulation for efficient urea electrosynthesis.\n                  <\/jats:p>","DOI":"10.1002\/anie.7521348","type":"journal-article","created":{"date-parts":[[2026,5,25]],"date-time":"2026-05-25T10:16:14Z","timestamp":1779704174000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":9,"title":["Reversing the Hydrogenation Pathways of Nitrogen\u2010Containing Intermediates for the Kinetics\u2010Matched Urea Electrosynthesis"],"prefix":"10.1002","volume":"65","author":[{"given":"Liwei","family":"Guo","sequence":"first","affiliation":[{"name":"MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage State Key Laboratory of Space Power\u2010Sources School of Chemistry and Chemical Engineering Harbin Institute of Technology  Harbin 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