• Gd3+ ions act as a microlevelling agent, preferentially adsorbing onto zinc protrusions to suppress dendrite growth.
• The adsorbed Gd3+ ions create a water-poor electric double layer, effectively inhibiting side reactions like hydrogen evolution and corrosion.
• The modified electrolyte enables zinc anodes to achieve a prolonged cycle life of 2100 hours and a high Coulombic efficiency of 99.72%.
• Full cells with NH4V4O10 cathodes demonstrate excellent capacity retention of 85.6% after 1000 cycles, highlighting practical applicability.
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