Chlorine is a critical element with respect to the use of fossil fuel, recycling of industrial wastes, and water purification. Chlorine could form toxic chemical compounds, corrode pipe systems and boilers, and contaminate surface and ground waters. Calcium aluminate-layered double hydroxides are one of the most promising materials to remove chlorides due to the chemisorption mechanism, since the phases have positively charged interlayers. Many studies on the synthesis and the characterization of calcium aluminate-layered double hydroxides have been extensively conducted, whereas few studies have been conducted on the chloride removal characteristics of the phases. The state-of-the-art studies on the synthesis methods and the structural characteristics of CaAl-LDH phases, the underlying mechanism on the removal of chlorides, and the potential removal rate and the capacity in the present study were thoroughly reviewed.