We employ molecular simulations to screen the best microporous materials for deep desulfurization of dry air. Pressure-swing adsorption and temperature-swing adsorption in desulfurization processes are investigated. The selectivity, working ability, selection parameters, and diffusivity of mixed gases are examined to evaluate those materials. The results show that UiO-66, ZIF-71, ZIF-69, and ZIF-97 exhibit good performance for the separation of H2S from air. The selectivity and adsorption capacity of H2S are larger than 300 and 0.01 mmol/g at room temperature and atmospheric pressure, respectively. UiO-66, ZIF-71, ZIF-69, MIL-100, Zn-DOBDC, ZnBDC, IRMOF-11, and MIL-140B are ideal materials to remove SO2 in air. The selectivity of SO2 is higher than 500 and the adsorption capacity is higher than 0.06 mmol/g. The diffusivity of sulfides is determined by the competition between the sterically hindered effect and the intermolecular synergistic effect. Comprehensive analysis found that zeolitic imidazolate frameworks (ZIFs) are good materials for the removal of sulfides.