Separating carbon dioxide (CO2) from gaseous streams released into the atmosphere is becoming critical due to its greenhouse effect. Membrane technology is one of the promising technologies for CO2capture. SAPO-34 filler was incorporated in polymeric media to synthesize mixed matrix membrane (MMM) and enhance the CO2separation performance of this process. Despite relatively extensive experimental studies, there are limited studies that cover the modeling aspects of CO2capture by MMMs. This research applies a special type of machine learning modeling scenario, namely, cascade neural networks (CNN), to simulate as well as compare the CO2/CH4selectivity of a wide range of MMMs containing SAPO-34 zeolite. A combination of trial-and-error analysis and statistical accuracy monitoring has been applied to fine-tune the CNN topology. It was found that the CNN with a 4-11-1 topology has the highest accuracy for the modeling of the considered task. The designed CNN model is able to precisely predict the CO2/CH4selectivity of seven different MMMs in a broad range of filler concentrations, pressures, and temperatures. The model predicts 118 actual measurements of CO2/CH4selectivity with an outstanding accuracy (i.e., AARD = 2.92%, MSE = 1.55, R = 0.9964).