The proton exchange membrane (PEM) is a fundamental component of the polymer electrolyte membrane fuel cell (PEMFC), a promising alternative energy conversion approach for low to medium power applications. Existing commercially available PEMs are based predominantly on perfluorosulfonic acid polymers (PFSA) (e.g., Nafion). In this study the viability of semi-interpenetrating ionomerpolymer networks from blends of poly(vinylidene fluoride) (PVDF) and covalently cross-linked sulfonated acrylic polyelectrolytes (PE) as potential PEMs is examined. A total of 80 PVDF/PE membranes, prepared from five different grades of Kynar PVDF (homo-and copolymers) and two types of PE, were characterized in terms of proton conductivity and mechanical properties using custom-developed high-throughput screening tools. In addition to PE type and content, the crystalline characteristics (i.e., crystallinity and crystallite size) and melt viscosity of the inert PVDF phase were found to have a major effect on proton conductivity. Particularly, membranes based on the most highly crystalline and viscous PVDF homopolymers exhibited the lowest proton conductivity, associated with reduced segmental motion of PE chains during membrane formation. Mechanical properties of the membranes were dominated by the properties of PVDF. Membranes based on higher modulus PVDF homopolymers exhibited higher elastic modulus and tensile strength, while those based on the more flexible poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF: HFP) copolymers exhibited enhanced toughness. In general, the resulting PVDF/PE membranes compared favorably to Nafion, having conductivities in excess of 130 mS/cm (vs 84.5 mS/cm for Nafion) and mechanical properties 2-5 times higher in some cases. While the selection of a unique conductivity and mechanical properties combination is impractical in view of the fact that requirements are dictated by the final application of the membrane, PVDF/PE semi-interpenetrated network membranes hold very good promise for PEMFC applications.