Dynamically Regulated Lithium Nucleation and Growth by Lithiophilic Seed Patterns With Laser‐Induced Gradient Edge for Stable Lithium Metal Anodes

ABSTRACT Lithium‐metal anodes promise high energy density but suffer from non‐uniform plating and dendrite growth. Here, we present a burr‐free, gradient‐edge lithiophilic seed patterning strategy on Ag‐coated Cu current collectors via near‐threshold Bessel‐beam laser ablation. This study establishes two fundamental design rules for stable lithium electrodeposition. First, the gradient‐edge topology significantly relaxes electric‐field hotspots, directing uniform Li nucleation and preventing early‐stage dendrite formation, as corroborated by finite‐element simulations. Second, systematically controlling the areal coverage of lithiophilic micro‐patterns modulates the local faradaic current density to precisely regulate Li nuclei density and size. This dynamic control sustains a smooth growth interface, revealing an optimal coverage window (∼45%–60%) that maximizes coulombic efficiency and minimizes interfacial impedance growth over cycling. At an optimized 45% coverage, nucleation overpotential drastically decreases to 30.9 mV (vs. 171.0 mV for bare Cu), maintaining compact Li deposits at 1.0 mAh cm −2 . When paired with LiFePO 4 cathodes in full cells, the patterned anodes exhibit superior rate capability and reduced voltage hysteresis (553 mV at 3 C). These findings highlight gradient‐edge lithiophilic patterning and coverage optimization as a scalable route for durable, high‐rate lithium‐metal batteries.