The oxygen reduction reaction (ORR) is central to modern energy storage and conversion technologies for grids such as fuel cells and electrolyzers, but challenges remain due to the lack of reliable, economic, and durable electrocatalysts. Here, we develop single‐crystal conductive black titanium (Ti4O7) nanosheets (NSs) as a new precious metal carrier based on sacrificial hard templates and ultrasonic‐assisted peeling, and deposit Pt clusters on Ti4O7  NSs induced by wetness impregnation under the irradiation of visible light (VI; 650 nm). Pt/Ti4O7  NSs provide Ti3+, Pt2+, and Pt0+ continuous active sites for the ORR multielectron process, achieving synergy among them. The assistance of visible light not only makes a more uniform and smaller distribution of Pt nanoclusters, but also strengthens the charge transfer, thereby constructing a strong metal‐support interaction interface. VI−Pt/Ti4O7  NSs show superior initial oxidation potential and a mass activity of 1.61 A mg−1Pt at a E1/2=0.91 V, which is nine times higher than that of commercial Pt/C. This work provides an effective strategy for achieving high‐value applications of titanium sub‐oxides and further explores the enhanced interface in metals TinO2n‐1 by light radiation.

The development of cost-effective and highly efficient electrocatalysts for water splitting is highly desirable but remains an ongoing challenge. Numerous single-atom catalysts (SACs) achieve satisfactory performances in this area, however,...

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Developing cost-effective electrocatalysts for the hydrogen evolution reaction (HER) is of great significance for renewable energy filed. Magnéli phase TinO2n-1 (4≤n≤10) has attracted much attention as promising carbon-free support for...