In cases of hollowing disease on roads, the interlayer hollowing form is relatively flat, and the cemented body tends to easily bend and fold after grouting repair. Additionally, the volume of roadbed hollowing is large, and the cemented body is prone to shrinking, leading to new diseases. Therefore, it is necessary to focus on improving the toughness, flexural strength, and shrinkage rate of the novel geopolymer grout repair material. Currently, there is a lack of grouting repair material tailored to these specific characteristics. This study presents the development of a novel geopolymer grouting repair material using slag and fly ash as the main raw materials. The brittleness of the novel material is improved by adding vinyl acetateethylene cogeopolymer (VAE) glue powder, and the flexural strength of it can also be improved. The shrinkage resistance of the material is improved by adding ultrafine fly ash microspheres. In addition, the effect of VAE and ultrafine fly ash microspheres on the performance of the grouting material was investigated. The novel geopolymer grouting material enhances road safety and durability by increasing flexural strength by 10.8%, reducing brittleness by 17.4%, and minimizing shrinkage by 38.2%. This is suitable for repairing interlayer hollowing disease on roads and promotes the advancement of road hidden disease repair technology.