Electrolyte nanocomposite membranes for proton exchange membrane fuel cells and direct methanol fuel cells were prepared by carrying out a sulfonation of poly(vinyl alcohol) with sulfosuccinic acid and adding a type of organically modified montmorillonite (layered silicate nanoclay) commercially known as Cloisite 93A. The effects of the different concentrations (0, 2, 4, 6, 8 wt. %) of the organoclay in the membranes on water uptake, ion exchange capacity (IEC), proton conductivity, and methanol permeability were measured, respectively, via gravimetry, titration, impedance analysis, and gas chromatography techniques. The IEC values remained constant for all concentrations. Water uptakes and proton conductivities of the nanocomposite membranes changed with the clay content in a nonlinear fashion. While all the nanocomposite membranes had lower methanol permeability than Nafion115, the 6% concentration of Cloisite 93A in sulfonated poly(vinyl alcohol) membrane displayed the greatest proton conductivity to methanol permeability ratio.