Today, the increasing world population has led to increased consumption of fossil fuels for energy production, causing environmental problems. Hydrogen with high energy density can be used as a suitable alternative to fossil fuel sources. Hydrogen atoms can be stored on porous structures by physical interaction. Hence, simple and eco-friendly approaches have been taken to prepare bentonite/Pd nanocomposites for electrochemical hydrogen storage. Laser ablation in the deionized water medium was employed as a physical route for the synthesis of Pd nanoparticles (NPs). Bentonite, a porous substrate with a high surface area of 47 m2/g, was employed for the deposition of Pd NPs via physical mixing. The morphological study of nanocomposite indicated that the spherically shaped Pd NPs with a diameter of 20–27 nm are successfully deposited on the bentonite substrate. The asprepared nanocomposites were loaded on stainless steel electrode through drop-casting and their hydrogen storage capacity was determined via cyclic voltammetry (CV). The CV measurement of the B/Pdx electrodes (x is laser ablation times of 15, 30, 45, and 60 min) in 1.0 M KOH electrolyte at the scan rate of 100 mV/s at room temperature demonstrated good hydrogen storage capacity (37 C/g) and stability during 200 scans.