Adsorption of gas mixtures is central to adsorption-based gas separations, and the number of adsorbate mixture/adsorbent systems that exist is staggering. Because examples of machine learning (ML) models predicting single-component adsorption of arbitrary molecules in large libraries of crystalline adsorbents have been developed, it is interesting to determine whether these models can accurately predict mixture adsorption. Here, we use molecular simulations to generate mixture adsorption data with a set of 12 near-azeotropic molecules in a diverse set of MOFs. These data provide a challenging example for any method to rapidly predict mixture adsorption in MOFs. We combine a previous ML single-component isotherm model with ideal adsorbed solution theory (IAST) to make predictions that can be compared directly with molecular simulation data for these adsorbed mixtures. This combination of ML and LAST illustrates the scope that is available with these methods, but the accuracy of the resulting predictions is disappointing. By examining the same examples with LAST based on minimal molecular simulation data for single-component isotherms, we show that having an accurate description of adsorption in the dilute loading limit is critical to being able to accurately predict mixture adsorption. This observation points to a useful direction for future work developing robust ML models of adsorption isotherms for diverse collections of molecules and adsorbents.