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Highly active and durable electrocatalysts are essential for producing hydrogen fuel through the hydrogen evolution reaction (HER). Here, a uniform deposition of Ru nanoparticles strongly interacting with oxygen-rich carbon nanotube architectures (Ru-OCNT) through ozonation and hydrothermal approaches has been designed. The hierarchical structure of Ru-OCNT is made by self-assembly of oxygen functionalities of OCNT. Ru nanoparticles interact strongly with OCNT at the Ru/OCNT interface to give excellent catalytic activity and stability of the Ru-OCNT, as further confirmed by density functional theory. Owing to the hierarchical structure and adjusted surface chemistry, Ru-OCNT has an overpotential of 34 mV at 10 mA cm À 2 with a Tafel slope of 27.8 mV dec À 1 in 1 M KOH, and an overpotential of 55 mV with Tafel slope of 33 mV dec À 1 in 0.5 M H 2 SO 4 . The smaller Tafel slope of Ru-OCNT than Ru-CNT and commercial Pt/C in both alkaline and acidic electrolytes indicates high catalytic activity and fast charge transfer kinetics. The asproposed chemistry provides the rational design of hierarchically structured CNT/nanoparticle electrocatalysts for HER to produce hydrogen fuel.

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