LAUSR

Conventional views of constructing simply broadband catalysts for photothermal‐enhanced catalysis do not realize that without designating photochemical and photothermal conversion to their optimal working spectra can lead to a performance trade‐off. Here, spectrally selective designed photoredox and photothermal heating functions of a classical oxide supported metal catalyst are demonstrated, which exhibits markedly improved hydrogen reactivity. While photothermal hydrogen producing catalysis is previously demonstrated, distinctive wavelength dominant redox and thermal phenomena are not studied due to the complex interdependent behavior they exhibit. The exceptionally high H2 evolution rate of 30.2 mmol g−1 h−1 (≈74 times that of the control sample) is attributed to the nonoverlapped light absorption and undisrupted charge transfer rationales. This study presents a proof‐by‐existence that spectrally tailored solar utilization strategy is broadly impactful for the hybrid photothermal–photochemical catalysis. Moreover, the spatially decoupled structural configuration may open up discrete parametric control over photoredox and photoheating functionalities.