Molecular simulations of binary adsorption in porous materials are a useful complement to experimental studies of mixture adsorption. Most molecular simulations of binary adsorption are performed using grand canonical Monte Carlo (GCMQ to independently examine a range of state points of interest. A disadvantage of this approach is that it only yields information at a discrete set of state points; therefore, if a complete isotherm is required for arbitrary conditions, some type of data fitting or interpolation must be used in combination with the GCMC data. We show that the transition matrix Monte Carlo (TMMC) method of Shen and Errington (Shen, V. K.; Errington, J. R. J. Chem. Phys. 2005, 122, 064508) is well-suited to simulation of binary adsorption in porous materials. At the completion of a TMMC simulation, the adsorption isotherm for all possible bulk phase compositions and pressures is available without data fitting or interpolation. It is also straightforward to use results from TMMC to compute derivatives of the isotherm such as the mixture thermodynamic correction factors, theta In fi/theta In c(j) again without data fitting or interpolation. This approach should be useful in contexts where information on the full adsorption isotherm is needed, such as the design of adsorption-or membrane-based separations.