Activated carbons of various origins (bituminous coal, wood, coconut shells, and peat) were studied as adsorbents of hydrogen sulfide. Before the experiments the surface of the adsorbents was characterized by using the sorption of nitrogen, Boehm and potentiometric titrations, thermal analysis, and FTIR. The adsorbents were chosen to differ in their surface areas, pore volumes, and surface acidities. To broaden the spectrum of surface acidity, carbons were oxidized by using nitric acid and ammonium persulfate. After hydrogen sulfide adsorption the species present on the surface were analyzed using thermal analysis, ion chromatography, and elemental analysis. The H2S breakthrough capacity tests showed that the performances of different carbons differ significantly. For a good performance of carbons as hydrogen sulfide adsorbents a proper combination of surface chemistry of carbon and porosity is needed. It was demonstrated that a more acidic environment promotes the formation of sulfur oxides and sulfuric acid despite yielding small H2S removal capacities. On the other hand, a basic environment favors the formation of elemental sulfur (sulfur radicals) and yields high capacities. The presence of a sufficient amount of water preadsorbed on the carbon surface to facilitate dissociation also plays an important role in the process of H2S adsorption/oxidation. The results showed that there is a critical value in carbon surface acidity, which when exceeded results in a negligible hydrogen sulfide breakthrough capacity. This is consistent with the mechanism of H2S adsorption on unmodified carbons, where the rate-limiting step is the reaction of adsorbed hydrogen sulfide ion with dissociatively adsorbed oxygen. When the acidity is expressed as pH, its value should be higher than 5 to ensure the effective removal of hydrogen sulfide from the gas phase. Study of carbon regeneration using water washing and heat treatment showed that the adsorbents can be regenerated to about 40% of their initial capacity.