Aqueous Zn ion batteries (ZIBs) are one of the most promising battery chemistries for grid-scale renewable energy storage. However, their application is limited by issues such as Zn dendrite formation and undesirable side reactions that can occur in the presence of excess free water molecules and ions. In this study, a nanocellulose-carboxymethylcellulose (CMC) hydrogel electrolyte is demonstrated that features stable cycling performance and high Zn2+ conductivity (26 mS cm−1), which is attributed to the material's strong mechanical strength (≈70 MPa) and water-bonding ability. With this electrolyte, the Zn-metal anode shows exceptional cycling stability at an ultra-high rate, with the ability to sustain a current density as high as 80 mA cm−2 for more than 3500 cycles and a cumulative capacity of 17.6 Ah cm−2 (40 mA cm−2). Additionally, side reactions, such as hydrogen evolution and surface passivation, are substantially reduced due to the strong water-bonding capacity of the CMC. Full Zn||MnO2 batteries fabricated with this electrolyte demonstrate excellent high-rate performance and long-term cycling stability (>500 cycles at 8C). These results suggest the cellulose-CMC electrolyte as a promising low-cost, easy-to-fabricate, and sustainable aqueous-based electrolyte for ZIBs with excellent electrochemical performance that can help pave the way toward grid-scale energy storage for renewable energy sources.https://doi.org/10.1002/adfm.20230209