standard hydrogen electrode (SHE)], natural abundance, and excellent safety of Zn anode, aqueous zinc-ion batteries (AZIBs) have recently attracted considerable research attention. [1][2][3][4] Nevertheless, dendrite growth, corrosion, and passivation at the anode-electrolyte interface hinder the widespread practical application of AZIBs. [5,6] Specifically, cumulatively grown dendrites pierce the separator, resulting in poor battery performance and even fire hazards. Additionally, the accumulation of insulating products through interfacial side reactions and the hydrogen evolution reaction (HER) at Zn anodes can severely reduce the coulombic efficiency (CE) and unevenly deposit Zn. [7][8][9][10] Hence, efficient measures are urgently required to protect Zn anodes.Recently, several strategies such as surface modification [11][12][13] and electrolyte manipulation [14][15][16][17][18] have been developed to solve these problems. Surface modification by creating a protective layer onto the Zn surface gains wide attention on account of the merits of simple and effective. [19] Previous studies have generally emphasized that protective layers have significant effect on promoting uniform Zn 2+ ion distribution and preventing direct contact of Zn anode with electrolyte, thereafter contributing to dendrite-free and side reactioninhibited Zn anode. [20][21][22][23][24] Going further, it should be pointed out that Zn 2+ ion exists as hydrated [Zn(H 2 O) 6 ] 2+ ion structure in aqueous electrolyte and the desolvation process is necessary before Zn deposition. [3] Moreover, the detrimental HER directly relates to the amount of free water at the electrode-electrolyte interface. Besides, the side reaction-resulted passiviation byproduct is usually Zn 4 SO 4 (OH) 6 •xH 2 O (ZSH) in ZnSO 4 electrolyte, [6,10] which simultaneously involves SO 4 2− ions and water molecules. This is to say, decreasing the number of SO 4 2− ions and free water near the Zn-electrolyte interface is significantly important in the side reaction-inhibited chemistry, which, however, has rarely attracted much attention. [27] In addition, noting that hydrated [Zn(H 2 O) 6 ] 2+ ions own high charge density and easily combine with anions, the desolvation penalty impedes the homogeneous Zn 2+ ion diffusion on the Zn anode. [25,26] In this regard, creating an artificial protective interface that simultaneously with good cation-selectivity and superior desolvation role is vitally important for homo geneous and kinetically enhanced Zn deposition, as well as side reaction-inhibited Zn anode.The Zn anode in aqueous zinc-ion batteries (AZIBs) is severely impeded by uncontrolled dendrite growth and promiscuous water-induced side reactions, resulting in low Coulombic efficiency (CE) and poor lifetime. Herein, a versatile Zn-based laponite (Zn-LT) interface is constructed for uniform and rapid Zn deposition for long-life AZIBs. The combined experimental results and theoretical simulations reveal that the abundant negatively charged channels in the Zn-LT layer permit cat...