With the development of phytoremediation of heavy metals contaminated soils, the harmless disposal of hyperaccumulator plants has been imminent. In this study, the effects of typical aluminosilicates on the heavy metal migration during the combustion of ryegrass were compared. The addition of kaolin, montmorillonite, and γ-Al2O3 were all effective in solidifying Pb and Zn. As the combustion temperature increased, the toxicity of remaining Pb and Zn decreased. Compared to montmorillonite, kaolin was more effective in capturing Pb and Zn at 600–825 °C, and the remaining Pb and Zn were mainly in acid-soluble form. The large amount of alkali/alkaline earth metals will react with the Si/Al components to form various potassium feldspars and calcium silicates, thus inhibiting the solidification of heavy/alkali metals. However, the Si in montmorillonite was more effective in converting Pb and Zn into residual form than kaolin when faced with the competition solidification of alkali/alkaline earth metals, at which time the percentage of Pb and Zn in the residual form increased from 13.27% and 6.00% to 39.21% and 9.84%, respectively. This work provided a research perspective based on the solidification of heavy metals by Si component, which enables a more comprehensive analysis of the differences in heavy metals solidification by Si/Al-based minerals.