Stacked Lamellar Matrix Enabling Regulated Deposition and Superior Thermo‐Kinetics for Advanced Aqueous Zn‐Ion System under Practical Conditions

Abstract Zinc anodes have attracted widespread attention for their intrinsic safety, low cost, and abundant resources, but still suffer from severe irreversibility due to spontaneous corrosion and nonplanar dendrite formation in aqueous electrolytes. In this work, a 3D stacked lamellar matrix (SLM) composed of ZnF 2 /Zn 3 (PO 4 ) 2 /CF X is elaborately designed on a Zn substrate via simple chemical/electrochemical reactions, delivering enhanced thermodynamic stability and rapid zinc ions transport kinetics. The abundant ion conduction channels in SLM could also redistribute Zn 2+ ions flux and further suppress the dendrite growth. With these synergetic effects, the SLM‐Zn anodes enable exceptional performance, including a high depth of discharge (90%) in a Zn|Zn symmetrical cell for 187 h, steady charge/discharge process (94.1% retention of SLM‐Zn|MnO 2 full cell for 1000 cycles at a harsh rate of 15 C), and low negative/positive capacity ratio (≈3.3) in SLM‐Zn|AC hybrid supercapacitor with limited Zn anode (10 µm) and high‐load cathode (≈1.77 mA h cm −2 ), which greatly promotes the application of aqueous Zn‐ion energy system under practical conditions.