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Existing reinforced concrete structures experience severe durability degradation when subjected to alkali– silica reaction (ASR) and chloride attack. A special electrochemical rehabilitation treatment, containing lithium compound anolyte, has been developed to drive lithium ions into concrete as well as remove chlorides simultaneously, for mitigating both the ASR-induced cracks and the chloride-induced corrosion. Good performance of introduced lithiums in controlling ASR-induced expansion has already been proved. Unfortunately, the migration mechanism of lithium in concrete under an external electric field is seldom investigated in existing literature. In this study, with help of the “double-multi” model, the efficiency of impregnation of lithium ions and simultaneously the removal of chloride ions through a specific electrochemical treatment are numerically evaluated, which results into the distribution profiles of all typical ionic species. The heterogeneous concrete model examines the aggregate effect, especially on the interaction with lithiums which are supposed to mitigate ASR. The ionic interaction between different species and the electrochemical reaction at electrodes are also considered. Through a relative thorough modelling of multi-phase and multi-species, a systemic parametric analysis based on a series of significant factors during electrochemical treatment (e.g., current density, treatment time, temperature, cathode position and concentration of lithium solution) reveals some important tendencies of ionic electromigration in concrete, which are supposed to guide the field application.