Composite chitosan/activated carbon hydrogels were prepared with the vapor-induced phase separation process. A rheometric study was performed with a factorial fractional design to determine the formulation and process parameters significantly influencing the mechanical properties of the gels. The results revealed that three factors played a key role in the storage modulus of the gels. According to the model, these factors could be classified with respect to their relative influence on the storage modulus in the following descending order: chitosan concentration > gel time of exposure to ammonia vapors > temperature of the reactor. Increasing these parameters led to an increase in the physical crosslinking density within the matrices and resulted in a reinforcement of the mechanical properties of the hydrogels. Two interactions were also shown to be significant and promoted the formation of supplementary junction zones within the matrix: the first one corresponded to the interaction between the chitosan concentration and the exposure time to ammonia vapors, and the second one concerned the interaction between the chitosan concentration and the temperature of the reactor. A second-order model was obtained from statistical analysis. Because of the determination coefficient (89.4%) and the P value related to the lack of adjustment of the model (0.043), which was associated with a 95% confidence level, this model could be considered to be of good quality. Three gels were used to validate the model, and good accuracy was obtained. The maximum elastic modulus was obtained with the highest chitosan concentration [4% (w/v)], the highest temperature in the gelation chamber (50 degrees C), and the longest time of exposure to ammonia vapors (24 h). (C) 2010 Wiley Periodicals, Inc. J Appl Polym Sci 120: 808-820, 2011