AbstractAqueous Zn metal‐based batteries have considerable potential as energy storage system; however, their application is extremely limited by dendrite development and poor reversibility. In this study, to overcome both challenges, F‐doped carbon nanoparticles (FCNPs) are uniformly constructed on substrates (Ti, Zn, Cu, and steel) by a plasma‐assisted surface modification, which endows reversible and uniform deposition of Zn metal. FCNPs with high surface charge density act as nucleation assistors and form numerous homogenous Zn nucleation sites toward Zn 3D growth, which improves Zn plating kinetic and results in uniform Zn deposition. Furthermore, the ZnF2solid electrolyte interface generated during cycling contributes to rapid mass transfer and enhances Zn reversibility, but also suppresses the side reaction. Accordingly, the half‐cell of P‐Ti coupled with Zn exhibits an average Coulombic efficiency of 99.47% with 500 cycles. The symmetric cell of the P‐Zn anode presents a lifespan of over 1500 h at the current density of 5 mA cm−2. Notably, the cell works for 100 h at 50 mA cm−2. It is believed that this ingenious surface modification broadens revolutionary methods for uniform metallic deposition, as well as the dendrite‐free rechargeable batteries system.