Rechargeable aqueous batteries are very attractive as a promising alternative energy storage system, although their reversible capacity is typically limited. A new rechargeable Na-Zn hybrid aqueous battery with nickel hexacyanoferrate (NiHCF) cathode and the nanostructured zinc anode is fabricated. The rational combination of two materials with mild aqueous electrolyte renders the devices with an average operating voltage close to 1.5 V, higher specific capacity of 76.2 mAh g−1, and a good cycling stability with 81% capacity retention for 1000 cycles. These remarkable features can provide guidance for the development of rechargeable batteries from the naturally abundant electrode materials with neutral aqueous electrolytes.