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The tensile stress–strain behavior of Nafion 117 and sulfonated poly(arylene ether sulfone) copolymer (BPSH35) membranes were explored with respect to the effects of the strain rate, counterion type, molecular weight, and presence of inorganic fillers. The yielding properties of the two films were most affected by the change in the strain rate. The stress–strain curves of Nafion films in acid and salt forms exhibited larger deviations at strains above the yield strain. As the molecular weight of the BPSH35 samples increased, the elongation at break improved significantly. Enhanced mechanical properties were observed for the composite membrane of BPSH35 and zirconium phenylphosphonate (2% w/w) in comparison with its matrix BPSH35 film. The stress‐relaxation behavior of Nafion and BPSH35 membranes was measured at different strain levels and different strain rates. Master curves were constructed in terms of plots of the stress‐relaxation modulus and time on a double‐logarithm scale. A three‐dimensional bundle‐cluster model was proposed to interpret these observations, combining the concepts of elongated polymer aggregates, proton‐conduction channels, and states of water. The rationale focused on the polymer bundle rotation/interphase chain readjustment before yielding and polymer aggregate disentanglements and reorientation after yielding. © 2006 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 44: 1453–1465, 2006