Cement-stabilized macadam (CSM) has been prevalently employed in transportation infrastructure owing to its superior bearing capacity and stability. However, with inherent dry shrinkage, temperature shrinkage, and inadequate tensile capacity, cracks will inevitably occur. These cracks can reflect on the asphalt layer and cause diseases such as transverse cracks, dynamic water scouring, voids, etc. A predominant remediation method involves utilizing grouting material for trenchless repair. In this research, a vinyl acetate-ethylene (VAE) latex modified superfine cement (VMSC) for grouting material is proposed to improve the flexibility of the grouting material and enhance crack repair dimensions. The interaction mechanism was investigated through mechanical experiments, microscopic tests, and molecular simulation. The results show that VMSC30 exhibits the highest fluidity. VAE latex addition extends the initial and final setting times of the grouting material, alongside an escalation in yield stress and plastic viscosity. VAE latex reduces the compressive strength of the grouting material, while 10% can increase the flexural strength, and the overall toughness can be improved. Characteristic spectral peaks of VAE latex are identified at 1740 cm−1 and 1240 cm−1, respectively, and it can form a film to cover the surface of cement, inhibit hydration diminish the CH peak value. VAE can form the 2.95 Å ionic bond and the 3.05 Å hydrogen bond on the Ca atom and water molecules, respectively. The peak value of the ionic bond is higher. The ionic bond and hydrogen bond formed by bridging can improve the strength of VAE and cement interfaces.