Molecular dynamics simulations have been performed to study the interfacial tension of CO2 and brine for a range of temperatures between 303 and 393 K and pressures from 2 to 50 MPa. The ions involved in this study are Na(+), Ca(2+), and Cl(-). The results indicate that the interfacial tension decreases with increasing pressure under any temperature condition but increases linearly with the molality of the salt solution. The density profiles calculated from the MD simulation results also indicate a positive excess of CO2 and a negative excess of ions at the interface. The charge of the ions was found to have a larger influence than their size on the interfacial tension, a result that consistent with experimental findings.