Artificial interfaces can alleviate the side reactions and the formation of the metallic (e.g., Li, Na, and Zn) dendrites. However, the traditional ones always breakdown during the repeated plating/stripping and fail to regulate the electrodeposition behaviors of the electrodes. Herein, a selfhealable ion regulator (SIR) is designed as a desolvation shield to protect the Zn electrodes and guide the Zn electrodeposition. Benefiting from the intermolecular hydrogen bonds, SIR shows a superb capability to in situ repair the plating/stripping-induced cracks. Besides, the results of theoretical calculations and electrochemical characterizations show that the coating reduces water molecules in the solvated sheath of hydrated Zn 2 + and restrains the random Zn 2 + diffusion on the Zn surface. Even with a coating layer of only 360 nm, the SIR-modified Zn electrode exhibits excellent long-term stability for > 3500 h at 2 mAh cm À 2 and > 950 h at an ultrahigh areal capacity of 20 mAh cm À 2 .