Femtosecond Laser Surface Processing (FLSP) is a versatile technique for the fabrication of a wide variety of micro/nanostructured surfaces with tailored physical and chemical properties. Through control over processing conditions such as laser fluence, incident pulse count, polarization, and incident angle, the size and density of both micrometer and nanometer-scale surface features can be tailored. Furthermore, the composition and pressure of the environment both during and after laser processing have a substantial impact on the final surface chemistry of the target material. FLSP is therefore a powerful tool for optimizing interfacial phenomena such as wetting, wicking, and phasetransitions associated with a vapor/liquid/solid interface. In the present study, we utilize a series of multiscale FLSPgenerated surfaces to improve the efficiency of vapor generation on a structured surface. Specifically, we demonstrate that FLSP of stainless steel 316 electrode surfaces in an alkaline electrolysis cell results in increased efficiency of the water-splitting reaction used to generate hydrogen. The electrodes are fabricated to be superhydrophilic (the contact angle of a water droplet on the surface is less than 5 degrees). The overpotential of the hydrogen evolution reaction (HER) is measured using a 3-electrode configuration with a structured electrode as the working electrode. The enhancement is attributed to several factors including increased surface area, increased wettability, and the impact of micro/nanostructures on the bubble formation and release. Special emphasis is placed on identifying and isolating the relative impacts of the various contributions.