Dry reforming of methane (DRM) with carbon dioxide to produce syngas is currently attracting a lot of attention for converting greenhouse gases into valuable chemicals. However, harsh reaction conditions in thermal catalysis hinder practical applications. Herein, a series of alumina‐supported NixFey nanoalloys are synthesized from NiFeAl‐layered double hydroxide precursors, with the obtained catalysts used for photothermal synergistic DRM. The Ni3Fe1 nanoalloy catalyst shows a syngas production rate of 0.96 mol g–1 h–1 under a 350 °C photothermal condition, which is about 1100 times higher than that of the same catalyst at the same temperature in the dark. Methane activation as the rate‐determining step in DRM is greatly enhanced by the localized surface plasmon resonance of the Ni3Fe1 nanoalloy in the ultraviolet region, thus accounting for the remarkably reduced reaction temperature. Meanwhile, the nanoalloy‐based photothermal synergistic DRM exhibits sunlight‐driven feasibility and 20 h of continuous operational stability.

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