Constructing a stable artificial solid-electrolyte interphase has become one of the most effective strategies to overcome the poor reversibility of lithium metal anode, yet the protection role is still insufficient at elevated current densities over 10 mA cm−2and large areal capacities over 10 mAh cm−2. Herein, we propose a dynamic gel with reversible imine groups, which is preparedviaa cross linking reaction between flexible dibenzaldehyde-terminated telechelic poly(ethylene glycol) and rigid chitosan, to fabricate a protective layer for Li metal anode. The as-prepared artificial film shows combined merits of high Young’s modulus, strong ductility and high ionic conductivity. When the artificial film is fabricated on a lithium metal anode, the thin protective layer shows a dense and uniform surface owing to the interactions between the abundant polar groups and lithium metal. Besides, the polar groups in the artificial film can homogenize the distribution of Li+at the electrode/electrolyte interface. As a result, cycle stability over 3200 h under an areal capacity of 10 mAh cm−2and a current density of 10 mA cm−2has been obtained for the protected lithium metal anodes. Moreover, cycling stability and rate capability has been also improved in the full cells.