This study addresses the issues of coarse primary austenite dendrites and uneven graphite distribution in hypoeutectic gray cast iron. High-energy mechanical activation technology was used to prepare high-energy activated SiC particles (EASiCp), and the regulatory mechanisms of trace additions (0–0.15 wt.%) on the solidification process and microstructure properties of hypoeutectic gray cast iron were systematically investigated. The results indicate that high-energy activation treatment reduced the average particle size of SiC particles from 26.53 μm to 9.51 μm and increased their specific surface area from 0.35 m²/g to 1.78 m²/g. X-ray diffraction (XRD) analysis revealed that the grain size was refined from 55.5 nm to 17.4 nm, with significant lattice distortion. The absorption rate of EASiCp in the melt stabilized between 68–72%, with particles predominantly dispersed within the grains (78.12%) and at grain boundaries (21.88%) in sizes ranging from 0.3 to 2 μm. The addition of EASiCp enhanced the solidification undercooling from 5.3 °C to 8.4 °C and reduced the latent heat of crystallization from 162.6 J/g to 99.96 J/g due to its endothermic reaction in the melt (SiC + Fe → FeSi + C) and heterogeneous nucleation effects. In terms of microstructure, the addition of 0.15 wt.% EASiCp increased the primary austenite dendrite content by 35.29%, reduced the secondary dendrite arm spacing by 57.98%, shortened the graphite length from 0.46 mm to 0.20 mm, and refined the eutectic colony size from over 500 μm to 180 μm. The final material achieved a tensile strength of 308 MPa, an improvement of 12.82% compared to the unadded group. Mechanistic analysis showed that EASiCp facilitated direct nucleation, reaction-induced “micro-area carbon enrichment,” and a synergistic effect in suppressing grain growth, thereby optimizing the solidification microstructure and enhancing performance. This study provides a new method for the efficient nucleation control of hypoeutectic gray cast iron.