Highlights The synergistic “anchor-capture” mechanism of polar groups on Zn stripping/plating process is firstly proposed. The amino group firmly anchors on Zn surface and the carboxyl group strongly captures Zn2+, constructing a robust anode–electrolyte interface and inducing uniform Zn deposition. The ultra-stable cycle lifespan of Zn–Zn symmetric cell (over 2800 h) and high utilization rate of Zn anode (the depth of discharge up to 68% for 200 h) are achieved under the proposal of synergistic “anchor-capture.”