Hydrogels composites composed of chitosan and activated carbon were prepared for medical applications using the vapor-induced phase separation process. Since the gelation process involves mass exchanges between the polymer solution and the air, the kinetics of mass transfer were investigated through experimental and modeling approaches. Among the formulation and process parameters, gravimetric measurements exhibited that mass transfers were mostly controlled by the initial ammonia partial pressure. A nonisotherm mass transfer model was developed to predict the nonsolvent and solvent exchange rates, therefore, the water and ammonia concentration profiles within the sample during the process. The numerical results were successively validated with gravimetrical kinetic curves obtained in a chamber where the process parameters were controlled. The model aimed also at predicting the pH moving front along the film thickness. The gelation time could also be predicted for differentoperating conditions (formulation and process parameters).