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Mechanical and electrochemical stability are key issues for large-scale production of solid state Li-ion batteries. Polymer electrolytes can provide good ionic conductivity, but mechanical strength needs to be improved. In this study, we investigate the correlation of mechanical and electrical properties of poly (ethylene oxide) (PEO)-based solid electrolytes for Li-ion batteries. The influence of alumina and LiClO₄ addition are investigated. Differential scanning calorimetry (DSC) is used to study the thermal behavior of salt-free and salt-containing samples and to identify the melting temperature. Dynamic mechanical analysis reveals the elastic properties as a function of temperature. Electrochemical properties are investigated using impedance spectroscopy. It is found that addition of alumina increases mechanical strength, while LiClO₄ decreases it. Addition of LiClO₄ and Al₂O₃ increases ionic conductivity and improves mechanical properties. However, there is no overlapping window of high mechanical strength and high ionic conductivity.