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Herein, a catalytic architecture consisting of nickel\u2010cobalt nanoclusters dispersed on gallium nitride nanowires supported by silicon for light\u2010driven hydrogen production from methanol is reported. By correlative microscopic, spectroscopic characterizations, and density functional theory calculations, it is revealed that NiCo nanoclusters work in synergy with GaN nanowires to enable the achievement of a significantly reduced activation energy of methanol dehydrogenation by switching the potential\u2010limiting step from *CHO \u2192 *CO to *CH\n                    <jats:sub>3<\/jats:sub>\n                    O \u2192 *CH\n                    <jats:sub>2<\/jats:sub>\n                    O. In combination with the marked photothermal effect, a high hydrogen rate of 5.62 mol\u00b7gcat\u20101\u00b7h\u20101 with a prominent turnover frequency of 43,460 h\u20101 is achieved at 5 Wcm\u20102 without additional energy input. Remarkably, the synergy between Co and Ni, in combination with the unique surface of GaN, renders the architecture with outstanding resistance to sintering and coking. The architecture thereby exhibits a high turnover number of &gt;16,310,000 over 600 h. Outdoor testing validates the viability of the architecture for active and robust hydrogen evolution under natural concentrated sunlight. Overall, this work presents a promising architecture for on\u2010site hydrogen production from CH\n                    <jats:sub>3<\/jats:sub>\n                    OH by virtually unlimited solar energy.\n                  <\/jats:p>","DOI":"10.1002\/smll.202309906","type":"journal-article","created":{"date-parts":[[2024,1,15]],"date-time":"2024-01-15T00:25:00Z","timestamp":1705278300000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":13,"title":["An Active and Robust Catalytic Architecture of NiCo\/GaN Nanowires\u00a0for Light\u2010Driven Hydrogen Production from Methanol"],"prefix":"10.1002","volume":"20","author":[{"given":"Jinglin","family":"Li","sequence":"first","affiliation":[{"name":"Key Laboratory for Power Machinery and Engineering of Ministry of Education Research Center for Renewable Synthetic Fuel School of Mechanical Engineering Shanghai Jiao Tong University  800 Dongchuan Road Shanghai 200240 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