Uniaxially prestretched recast Nafion membranes exhibited an unusual combination of properties (a proton conductivity equal to that of commercial Nafion but with a lower methanol permeability) which make them ideal candidates for use in a direct liquid methanol fuel cell. To better understand the function and underlying morphology of the prestretched membranes, water uptake and mobility data were collected and analyzed for draw ratios ranging from 1 to 7. Macroscopic (gravimetric) water uptake and the water self-diffusion coefficient (measured by NMR) were found to be invariant with membrane elongation and essentially identical to those measured in a commercial Nafion 117 film (a similar behavior was observed for proton conductivity). The ratio of freezable/nonfreezable water in prestretched recast Nafion, the water electro-osmotic drag coefficient, and the spin-lattice relaxation time constant of deuterated water, however, decreased with increasing film elongation, up to a draw ratio of 4. The functional dependence of these properties on draw ratio was similar to that observed for methanol permeability. The combined water results indicated that there were a greater number of smaller ionic/hydrophilic domains in prestretched recast Nation as compared to commercial Nafion. Transmission electron microscopy of membrane cross sections confirmed this conclusion.