Abstract: It is acknowledged that injecting CO2 into oil reservoirs and saline aquifers for storage is a practical and affordable method for CO2 sequestration. Most CO2 produced from industrial exhaust contains impurity gases such as H2S that might impact CO2 sequestration due to competitive adsorption. This study makes a commendable effort to explore the adsorption behavior of CO2/H2S mixtures in calcite slit nanopores. Grand Canonical Monte Carlo (GCMC) simulation is employed to reveal the adsorption of CO2, H2S as well as their binary mixtures in calcite nanopores. Results show that the increase in pressure and temperature can promote and inhibit the adsorption capacity of CO2 and H2S in calcite nanopores, respectively. CO2 exhibits stronger adsorption on calcite surface than H2S. Electrostatic energy plays the dominating role in the adsorption behavior. Electrostatic energy accounts for 97.11% of the CO2-calcite interaction energy and 56.33% of the H2S-calcite interaction energy at 10 MPa and 323.15 K. The presence of H2S inhibits the CO2 adsorption in calcite nanopores due to competitive adsorption, and a higher mole fraction of H2S leads to less CO2 adsorption. The quantity of CO2 adsorbed is lessened by approximately 33% when the mole fraction of H2S reaches 0.25. CO2 molecules preferentially occupy the regions near the pore wall and H2S molecules tend to reside at the center of nanopore even when the molar ratio of CO2 is low, indicating that CO2 has an adsorption priority on the calcite surface over H2S. In addition, moisture can weaken the adsorption of both CO2 and H2S, while CO2 is more affected. More interestingly, we find that pure CO2 is more suitable to be sequestrated in the shallower formations, i.e., 500–1500 m, whereas CO2 with H2S impurity should be settled in the deeper reservoirs.