Interfacial Nucleation Processes With SEI Governed for Zinc Ion Batteries

ABSTRACT Understanding the zinc nucleation and growth process is crucial for improving zinc metal battery performance. While both the solid‐electrolyte interphase (SEI) and the substrate are known to influence zinc nucleation, their respective roles and interplay remain quantitatively far from clear. Here, we decouple these interactions by constructing an organic–inorganic hybrid SEI, while SEI properties make the zinc nucleation and growth controlled by SEI and substrate independent. This SEI‐induced control mechanism directs zinc to preferentially nucleate along the (101) crystal plane, achieving ordered plating/stripping and effectively suppressing dendrite formation. Consequently, we achieved exceptionally stable zinc electrodeposition, enabling symmetric Zn//Zn cells to deliver an ultra‐long cycling life of over 6000 h at 0.25 mA cm − 2 . These findings resolve a fundamental debate in interfacial electrochemistry and provide a universal design principle for sustainable energy storage systems.