This study investigates mixtures of water and cryoprotectant agents (CPAs) to store high-grade cold energy. Although water is an ideal material for a cold thermal storage (CTS) due to its high specific heat, undesirable volume expansion may cause structural stresses during freezing. The volume expansion can be alleviated by adding the CPAs to water. However, the CPA aqueous solutions not only have different thermal properties but also transit to amorphous state different from pure water. Therefore, these characteristics should be considered when using them as material of the CTS. In experiments, glycerol and dimethyl sulfoxide (DMSO) are selected as the candidate CPA. The volume expansion of the solution is measured by an in-situ strain gauge in low temperature region. The specific heat capacity of the solution is also measured by differential scanning calorimetry (DSC). Both the amount of volume expansion and the specific heat capacity of the CPA aqueous solution decrease in the case of higher concentration of CPA. These characteristics should be contemplated to select optimal aqueous solution for CTS for liquid air energy storage system (LAES). The CPA solutions have advantages of having wide temperature range to utilize the latent heat of water and higher sensible heat of the CPA. The CPA solutions which can satisfy the allowable stress of the structure are determined. Consequently, among the CPA solutions investigated, DMSO 20% w/w solution is the most suitable for the CTS.