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Polymer electrolytes have potential for use in solid state electrochemical devices owing to favorable material properties. We have developed a multifunctional concept for material development that integrates structural performance with energy storage. One focus of our research is to develop polymer electrolytes that exhibit a desirable combination of mechanical strength and ion conductivity. In the present study, PEG vinyl esters were complexed with lithium triflate and studied as both homopolymer and random copolymer electrolytes. Lithium content was first optimized on a diverse sampling of the set through varied salt concentrations. Homopolymer electrolytes at 30 EO:Li were then characterized. The homopolymers vary in length of PEG oligomers, number of vinyl esters per monomer, and additional functionality. Random copolymer electrolytes were investigated using electrochemically strong monomers and mechanically strong monomers in systematically varied weight percent. The resulting electrochemical and mechanical properties will be discussed as well as the directions of future research., Reprinted from Proceedings of the American Chemical Society Division of Polymeric Materials: Science & Engineering (PMSE Preprints), V93, Fall 2005, Washington, D.C., 28 Aug-1 Sep 2005. The original document contains color images.