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This study developed a new electrodeposited Fe–Ni coatings using the laser-induced current waveform. This process refined grains accomponied with a mixed nanocrystalline size and alternate element content. The electrochemical and immersion corrosion performance at 3.5 wt% NaCl was improved, which is still pitting corrosion. The corrosion pits are more likely to spread around rather than in the depth direction. The enhancement mechanism is mainly attributed to the richer grain boundaries. This microstructure increases the interface transfer resistance and makes the corrosion more uniform. This study provides a potential process for preparing nanocrystalline coatings with better performance. [Display omitted] • Laser-induced current waveform refines grains with a mixed size. • The element content is distributed alternately along the cross-section. • The electrochemical and immersion corrosion properties are improved. • The enhance mechanism is mainly attributed to the rich grain boundaries. [ABSTRACT FROM AUTHOR]