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In this study, the chloride adsorption behaviors of CaAl-Cl LDH precursors with various Ca:Al ratios were investigated. The optimal chloride ion removal rate was 87.06% due to the formation of hydrocalumite. The chloride adsorption products of CaAl-Cl LDH precursors were further characterized by X-ray diffraction analysis and atomic structure analysis, the adsorption mechanism was considered to be co-precipitate process. The chloride adsorption behaviors of cementitious materials blended with CaAl-Cl LDH precursors were further investigated. Leaching test according to Test Code for Hydraulic Concrete (SL352-2006) was performed to testify the stability of chloride ions in the mortar. The results show that more than 98.3% chloride ions were immobilized in cement mortar blended with CaAl-Cl LDH precursor and cannot be easily released again. The inhibition performance of steel in the electrolytes with/without CaAl LDH precursor was investigated by using electrochemical measurements. The results indicate that CaAl LDH precursor can effectively protect the passive film on steel surface by chloride adsorption. Considering the high anion exchange capacities of the LDHs, synthesized chloride adsorbent precursor can be applied as new inhibitors blended in cementitious materials to prevent the chloride-induced deterioration. Moreover, the application of chloride adsorption on CaAl-Cl LDH could also be of interest for the application of seawater blended concrete.