Despite their low cost, safety, environmentally friendliness, and intrinsic non‐flammable nature, the widespread application of aqueous rechargeable zinc‐based batteries has been held back by their low coulombic efficiency and the notorious dendritic growth at the zinc‐based anodes, along with the fast capacity fading of the cathodes. Herein, an aqueous Zn superbattery that consists of a mixed ZnCO3 MnCO3 grafted onto a graphene aerogel (ZMG) negative electrode and a nanotubular sulfidated NiCoFe layered double hydroxide (LDHS) positive electrode is reported. The alkaline ZMG││LDHS superbattery delivers an excellent capacity and a superb rate capability (356 mA h g−1cathode (89 mA h g−1total mass) at 12 A g−1; 108 mA h g−1cathode at 300 A g−1), extremely high specific energy and power (568 W h kg−1cathode or 15.8 mW h cm−3, 429 kW kg−1cathode or 11.9 W cm−3), along with a high output voltage (1.8 V). The device also exhibits unprecedented cycling stability (99.2% capacity retention after 17,000 cycles at 100% depth of discharge) thanks to an electrochemical pulse‐driven regenerative mechanism.
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