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Developing highly efficient catalysts using facile approaches is important for accelerating the slow reaction kinetics of the alkaline hydrogen evolution reaction (HER) and ensuring cost-effective hydrogen production. In this study, we reported a facile alkali etching method to boost the HER activity immediately after electrodeposition of a NiFeZn catalyst on Ti paper. During etching, (oxy)hydroxides were formed on the surface, and Zn species were etched from the deposits, which resulted in a roughened surface with more valleys generated between grains, facilitating a faster mass transport during the electrochemical reaction. The etched catalyst exhibited a boosted HER overpotential of 57 mV at −10 mA/cm2 and accelerated HER kinetic with Tafel slope of 97 mV/dec compared with that of the pristine catalyst. Our results demonstrated an efficient approach for boosting the catalyst activity in the alkaline HER. [Display omitted] • NiFeZn electrocatalysts were prepared on Ti paper using electrodeposition method. • Their morphology and composition were controlled by varying deposition potential. • An alkali etching method is proposed to boost the pristine NiFeZn electrocatalyst. • The defect surface of NiFeZn generated by alkali etching improved HER activity. [ABSTRACT FROM AUTHOR]