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Thermally reversible self-healing polymer (SHP) electrolyte membranes are obtained by Diels-Alder cycloaddition and electrolyte embedding. The SHP electrolytes membranes are found to display high ionic conductivity, suitable flexibility, remarkable mechanical properties and self-healing ability. The decomposition potential of the SHP electrolyte membrane is about 4.8 V (vs. Li/Li⁺) and it possesses excellent electrochemical stability, better than that of the commercial PE film which is only stable up to 4.5 V (vs. Li/Li⁺). TGA results show that the SHP electrolyte membrane is thermally stable up to 280 °C in a nitrogen atmosphere. When the SHP electrolyte membrane is used as a separator in a lithium-ion battery with an LCO-based cathode, the SHP membrane achieved excellent rate capability and stable cycling for over 100 cycles, and the specific discharge capacity could be almost fully recovered after self-healing. Furthermore, the electrolyte membrane exhibits excellent electrochemical performance, suggesting its potential for application in lithium-ion batteries as separator material.