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Amorphous materials can serve as an effective support matrix to form unique crystalline\u2010amorphous interfaces and modulate the electronic structure of active metals. However, robust synthetic strategies for precise structural control remain underdeveloped. Here, we report the laser\u2010shocked synthesis of heterostructures including bimetallic CuNi, CuFe, CuCo, and medium\u2010entropy CuFeCoNi heterostructures, where crystalline metal nanoparticles are anchored on amorphous hydroxide supports. The heterostructures are characterized by an interfacial electronic distribution that improves catalytic activities. With CuNi as an example for nitrate reduction reaction, the laser\u2010engineered heterophase CuNi achieves an NH\n                    <jats:sub>3<\/jats:sub>\n                    production rate of 92.18\u00a0mg\/h\/mg\n                    <jats:sub>cat<\/jats:sub>\n                    with 98.6% Faradaic efficiency (FE), substantially superior to standalone crystalline CuNi or amorphous CuNi hydroxide. The CuNi heterostructure maintains a stable FE(NH\n                    <jats:sub>3<\/jats:sub>\n                    ) of \u223c90% up to 80\u00a0h while improving current density from 75 to 120\u00a0mA\/cm\n                    <jats:sup>2<\/jats:sup>\n                    due to the robust amorphous layer and dynamic amorphous\/crystalline reconstruction. In situ characterization and theoretical calculations reveal that the amorphous\/crystalline interface regulates the balance between reactive hydrogen species and reaction intermediates, effectively suppressing the competing hydrogen evolution and promoting cascade nitrate\u2010to\u2010nitrite and nitrite\u2010to ammonia conversion. This work provides a general and viable strategy for producing high\u2010performance supported catalysts.\n                  <\/jats:p>","DOI":"10.1002\/adma.73764","type":"journal-article","created":{"date-parts":[[2026,6,19]],"date-time":"2026-06-19T06:04:46Z","timestamp":1781849086000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Transient Laser\u2010Shocked Synthesis of Amorphous Layer\u2010Supported Metal Nanocrystals for Efficient Nitrate Reduction"],"prefix":"10.1002","volume":"38","author":[{"given":"Weihua","family":"Guo","sequence":"first","affiliation":[{"name":"Department of Chemistry State Key Laboratory of Marine Pollution City University of Hong Kong  Hong Kong China"},{"name":"City University of Hong Kong Shenzhen Research Institute  Shenzhen Guangdong 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