Wulff‐Guided (002)/(103) Faceted Step–Terrace Microtopography Enables Rapid and Reversible Zn Deposition

ABSTRACT Controlling Zn crystallographic orientation provides an effective pathway to stabilize Zn metal anodes. However, conventional single‐textured Zn anodes face an intrinsic trade‐off between interfacial stability and deposition kinetics. Herein, we develop an ion co‐driven Wulff‐guided crystal growth strategy to construct a step–terrace Zn microtopography consisting of (002) terraces and (103) step facets. The Zn 2+ concentration regulates Zn growth kinetics, while preferential adsorption of H + /SO 4 2− selectively modifies facet dependent surface energies to reshape the Wulff construction. The (002)/(103) step–terrace interface exhibits synergistic advantages. The (002) terraces enhance interfacial stability through HER suppression, while the (103) steps and activated (002) terrace edges accelerate Zn nucleation and interfacial kinetics. This ordered step–terrace architecture enables spiral Zn growth, leading to uniform and dendrite free Zn deposition. Consequently, the step–terrace Zn anode maintains a Coulombic efficiency of 99.80% for 2000 h and enables stable Zn plating/stripping for 500 h at 5 mA cm −2 with 50% depth of discharge. Full cells retain 313.0 mAh g −1 after 8000 cycles at 10 A g −1 , corresponding to a decay rate of 0.0022% per cycle. This work establishes a Wulff‐guided step–terrace interface paradigm for long‐life aqueous zinc‐ion batteries.