Laser ablation is a scalable technique for decreasing the effective tortuosity of electrodes by selectively removing material with high precision. Applied to ? 110 um thick electrode coatings, this work focuses on understanding the impact of laser ablation on electrode material properties at the beginning of life and synergistic impacts of ablated channels on cell performance throughout their cycle life. Post laser ablation, local changes in chemistry, crystallography, and morphology of the laser-impacted electrode regions are investigated. It is shown that femtosecond pulsed laser ablation can achieve high-rate material removal with minor material damage locally at the interface of the impacted zones. The capacity achieved during a 6C (10 min) constant-current constant-voltage charge to 4.2 V improved from 1 mAh cm<
sup>
-2<
/sup>
for the non-ablated electrodes to almost 2 mAh cm<
sup>
-2<
/sup>
for the ablated electrodes. This benefit is attributed to a synergistic effect of enhanced wetting and decreased electrode tortuosity. The benefit was maintained for over 120 cycles, and upon disassembly decreased Li-plating on the graphite anode was observed. Finally, multi-physics modeling in conjunction with wetting analyses showed that laser ablating either one of the electrodes led to substantial improvements in wetting and rate capability, indicating that substantial performance benefits can be achieved by ablating only the graphite anode as apposed to both electrodes.