Sulfoaluminate cement-based materials (SCBMs) are widely used for grout reinforcement. It is common to use a large water-to-binder ratio in the construction of sulfoaluminate cement-based materials (SAGMs) to obtain good workability and permeability, which results in poor early strength. Nanotechnology has been increasingly employed to enhance the mechanical properties of cementitious materials. Nano Zn-Mg-Al hydrotalcite-like (LDHs) and nano Mg-Al LDHs increased the early compressive strength, while nano Zn-Al LDHs had the opposite effect. However, the reason for this observation remains unclear. In this study, the influence of LDHs structures with different laminar element compositions on the hydration and hardening processes of SCBMs was analysed. The results showed that nano-ZnAl-LDHs, ZnAl-LDHs, and MgAl-LDHs could provide nucleation sites for ettringites. The three hydrotalcite-like materials slowly released different concentrations of zinc and/or magnesium ions and carbonate ions in the cement paste. Zinc ions entered the hydration product of ettringite and aluminum gel and promoted the transformation of amorphous aluminum gel to bayerite, which inhibited the hydration reaction of SCBMs. Magnesium ions could also enter the ettringite, and carbonate ions promoted the formation of calcium carbonate, which facilitated the hydration reaction of SCBMs. The nucleation effect and the release of zinc and/or magnesium ions and carbonate ions acted synergically to influence the hydration rate, pore size distribution, and compressive strength of SCBMs.