The present study examines the interaction of hydrogen and nitrogen plasmas with gallium in an effort to gain insights into the mechanisms behind the synergetic effect of plasma and a catalytic metal. Absorption/desorption experiments were performed, accompanied by theoretical-computational calculations. Experiments were carried out in a plasma-enhanced, Ga-packed, batch reactor and entailed monitoring the change in pressure at different temperatures. The results indicated a rapid adsorption/dissolution of the gas into the molten metal when gallium was exposed to plasma, even at a low temperature of 100 °C. The experimental observations, when hydrogen was used, indicate that gallium acts as a hydrogen sink in the presence of plasma. Similar results were obtained with Ga in the presence of nitrogen plasma. In addition, density functional theory calculations suggest a strong interaction between atomic hydrogen and molten gallium. This interaction is described as a high formation of Ga-H species on the surface, fast diffusion inside the metal, and a steady state concentration of the gas in the bulk.