• A bilayer of zincophilic Cu and flexible polymer on Zn anode enables uniform Zn deposition and suppresses dendrites.
• The Cu layer provides nucleation sites, while the polymer layer prevents side reactions, enhancing cycle stability.
• Symmetric cells achieve over 2900 h cycling at 1 mA cm−2, and full cells retain 72% capacity after 500 cycles.
• This strategy offers a simple, effective approach to improve aqueous zinc-ion battery performance for practical applications.
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