Prediction of mixed gas adsorption by the multisite Langmuir (MSL) theory is significantly improved by incorporating the multiregion adsorption (MRA) theory. The new model, called the multiregion multisite Langmuir (MR-MSL) model, is thermodynamically consistent. MR-MSL uses the same pure-component isotherm parameters as MSL does, and no new parameters are introduced. Eight binary systems and one ternary system are used to test the MR-MSL model. For systems containing like components (such as mixtures of hydrocarbons and that of O-2 + N-2), MR-MSL yielded only minor improvements over MSL. This is true regardless of the magnitude of the differences in the pure-component MSL parameters among different components. For highly nonideal mixtures, MR-MSL results in very substantial improvements. It is also capable of predicting the azeotropic behavior of the adsorption of CO2 + C3H8 on H-mordenite and the correct azeotropic compositions. For such systems, it is also shown that surface heterogeneity needs to be considered.