Yes / The inclusion of crystalline admixture (CA) is a highly effective method for enhancing the self-repairing capabilities of mortar. This study examined the complexing abilities of different complexing agents under varying temperatures, pH levels, and ion species in order to select effective complexing agents for diverse environments, as complexing agents play a crucial role in CAs. After determining the type of complexing agent, an orthogonal array design was used to optimize the components of CA, and the strengthening mechanism of CA for mortar was discussed through microstructure analysis. The results showed that the complexation behavior of triethanolamine (TEA) and glycine performed better than sodium citrate (SC) for different pH, temperatures, and ion species. Meanwhile, TEA and glycine showed complementarity at different stages, so TEA and glycine were used as complexing agents in this study. Based on the orthogonal experiment, the optimal contents of Na2SiO3, Na2CO3, TEA, glycine, Ca(COOH)2, and nano-SiO2 in CA were determined to be 1.0%, 1.0%, 0.04%, 1.0%, 0.5%, and 1.0%, respectively. Under the synergistic effect of TEA and glycine, the hydration of aluminate and ferrialuminate was accelerated, and the hydration degree of cement paste was increased. At 28 d, the contents of CaCO3, C-S-H gel, and ettringite of cement paste with CA were higher than these of plain paste, but its Ca(OH)2 content was lower. Although the Ca(OH)2 content in the cement paste with CA was lower, the Ca(OH)2 crystal structure filled in the pores was larger. Therefore, the mortar mixed with CA exhibited higher compressive strength, water impermeability, and self-healing ability. / The full-text of this article will be released for public view at the end of the publisher embargo on 3 May 2025.