Cerium oxide (CeO2) nanoparticles are widely used as abrasives in chemical mechanical polishing (CMP), an essential process for obtaining Si wafers with excellent surface quality. While CeO2 nanoparticles form Ce–O–Si bonds, which exhibit good CMP performance, their low activity results in a low removal rate. To address this issue, a two-step ultrasonic dispersion method was employed to prepare a uniform nuclear@shell CeO2@ZIF-8. The process of chemical bond generation in CMP was studied using spherical aberration-corrected transmission electron microscopy and X-ray photoelectron spectroscopy. In comparison to pure cerium oxide, the formation of Ce–O–Si bond was observed, and notably, the emergence of N–Si bond originating from the N of the ZIF-8 shell was identified. Coupled with the increased Ce3+ content, these developments enhanced CMP performance. The material removal rate (MRR) of the CeO2@ZIF-8 abrasives was 151.507 nm/min, which is 89.72 % higher than that of the pure CeO2 abrasives. Moreover, the surface roughness, as determined via AFM testing, was reduced to 0.231 nm within the confines of a 5.0 × 5.0 μm² region. Therefore, this study introduces a novel concept for CMP research by developing a CeO2@ZIF-8 compound abrasive to create a new N–Si bond.