Acrylic materials exhibit favorable grouting repair performance. However, their curing products are easily inclined to drying shrinkage, and their concrete impermeability repair characteristics have seldom been investigated. To improve material properties, reveal the impermeability repair mechanism, and address drying shrinkage, this study proposed the addition of styrene–acrylate copolymer emulsion (styrene–acrylic emulsion) to the grouting material to prepare two-component acrylate grouting materials. Using orthogonal and single-factor tests combined with physical and mechanical properties, the mechanical properties and impermeability repair performance (physical and mechanical properties combined) of grouting materials were analyzed and studied, and the optimal ratio of each component of acrylate grouting materials was determined. Results show that (1) the hydrogel produced by the reaction of sodium methacrylate with hydroxyethyl acrylate has good physical and mechanical properties. (2) With the increase in the accelerator dosage, the setting time of slurry initially decreases and then increases; as the initiator dosage increases, the setting time of slurry decreases, which is negatively correlated with the initiator dosage. (3) Talcum powder can improve the physical and chemical properties of gel and enhance the reliability and durability of acrylate grouting materials, and the comprehensive performance is the best at a dosage of 3%. (4) Styrene–acrylic emulsion can increase the solid content and reduce the volume drying shrinkage when added to grouting materials. The fractured impermeable specimens were repaired by grouting with prepared acrylate grouting materials and cured for 24 h for the impermeability test, and the water pressure for the 24 h impermeability repair was 1.0 MPa. This study’s results provide important reference and basis for revealing the impermeability principle of acrylate grouting materials and evaluating their impermeability.