The severe hydrogen evolution reaction and parasitic side reaction on Zn anode are the key issues which hinder the development of aqueous Zn-based energy storage devices. Herein, a polyacrylamide/carboxylated cellulose nanofibers/betaine citrate supramolecular zwitterionic hydrogels with molecular slip effects are proposed for enhancing Zn 2+ diffusion and protecting Zn anodes. Non-covalent interactions within supramolecular hydrogels forms the skeleton for molecular slip and the strong coordination of carboxyl and amino groups with Zn 2+ further facilitates the rapid Zn 2+ transfer. Additionally, anchoring carboxyl and amino groups at the anode promotes the uniform deposition of Zn 2+ and protects Zn anode. On the basis of molecular slip mechanism and anchoring effect in the supramolecular zwitterionic hydrogels, Zn||Zn symmetric batteries undergo 800 h of stable electroplating stripping at a depth of discharge of 80 %. Zn||Cu asymmetric batteries exhibit an impressive average coulombic efficiency of 99.4 % over a remarkable span of 900 cycles at a current density of 15 mA cm -2 . Furthermore, Zn||NH 4 V 4 O 10 batteries successfully undergo over 1,000 cycles at a current density of 0.5 A g -1 . Intrinsic ion diffusion mechanism of supramolecular hydrogel electrolytes provides an original strategy for the application of high-performance Zn-based energy storage devices.