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Designing and synthesis of cost-effective and improved methanol permeable and proton conductive membranes are the main challenges for preparation of polymeric electrolyte membrane (PEM). Herein, a cost-effective PEM membrane based on phosphorylated polyvinyl alcohol (PVA)-grafted-cellulose acetate (CA) was prepared by a solution-casting technique. Water and methanol uptakes of phosphorylated PVA/CA membranes were characterized as function with the molar ratio of CA. Additionally, structure and morphology of phosphorylated PVA/CA (Ph-PVA/CA) membranes were verified by FT-IR analysis, SEM investigation. Furthermore, ion exchange capacity (IEC), proton conductivity and methanol permeation of Ph-PVA/CA membranes were examined based on the concentration of OPA basically. The results manifested a perceptible improvement in proton conductivity from 0.035 to 0.05 S/cm at 25 and 70 °C, respectively using 600 μL of OPA, and IEC of 2.1 meq/g using 400 μL of OPA at ambient temperature. On the other hand, methanol permeability (P = 1.08 × 10–10 cm2/s) was lower than Nafion 117 admirably. The optimum OPA concentration was 200 μL according to conductivity measurements (at 10% PVA, 150 μL GA, and CA 7%). Finally, prepared Ph-PVA/CA membranes exhibited enhancement in critical natures such as proton conductivity and IEC combined with its low-cost materials, which make them excellent candidate as PEM for DMFCs application. [ABSTRACT FROM AUTHOR]