Cement grouting material is one of the most important materials in civil construction at present, for seepage prevention, rapid repair, and reinforcement. To achieve the ever-increasing functional requirements of civil infrastructures, cement grouting materials must have the specific performance of high fluidization, early strength, and low shrinkage. In recent years, nanomaterials have been widely used to improve the engineering performance of cement grouting materials. However, the mechanisms of nanomaterials in grouting materials are not clear. Hence, a high-fluidization, early strength cement grouting material, enhanced by nano-SiO2, is developed via the orthogonal experimental method in this study. The mechanisms of nano-SiO2 on the microstructure and hydration products of the HCGA, in the case of different curing ages and nano-SiO2 contents, are analyzed through scanning electron microscopy tests, X-ray diffraction tests, differential scanning calorimetry tests, and Fourier transform infrared spectroscopy tests.