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This study describes the fabrication of ultrafast laser-induced periodic nanostructures on Nickel sheets and their use as cathodes in alkaline electrolysis. For the first time, to the best of our knowledge, laser-nanostructured Ni sheets were used as cathode electrodes in a custom-made electrolysis cell at actual, Hydrogen producing conditions, and their efficiency has been compared to the untreated Nickel sheets. The electrochemical evaluation showed higher J peaks , lower overpotential, and enhanced double-layer capacitance for the nanostructured electrode. A decrease in the Tafel slope was also found for the nanostructured electrode. The hydrogen production efficiency was found to be 3.7 times larger for the laser-nanostructured Nickel electrode, which was also confirmed by current-time measurements during electrolysis. Also, a novel approach is proposed to improve the stability of the current density during electrolysis and, therefore, the hydrogen production process by about 10%. [Display omitted] • Laser nanostructured Ni electrodes produce higher values of hydrogen gas. • An Electrochemical evaluation of laser nanostructured Ni electrodes. • A Correlation between electrical measurements and hydrogen production during electrolysis. [ABSTRACT FROM AUTHOR]