Molecular dynamics has been used to study possible dynamic mechanisms that may contribute to the property degradation known to exist for polybenzimidazole (PBI) upon hydration. During this study, chaotic movements of a chain pair were observed. Changes in onset and duration of this movement were also observed, which depended upon both hydration state and stress direction involved. Such trends suggested that specific mechanistic pathways may exist that could directly lead to property (such as modulus) loss.