The continuous reduction in feature size of integrated circuits has raised stricter material removal selectivity and surface quality requirements for the chemical mechanical polishing (CMP) process of shallow trench isolation (STI). To reduce surface defects, small-sized CeO2 abrasives are introduced into the CMP of STI. We investigated the impacts of three amino acids and their composites added to a 50 nm-sized CeO2 dispersion (pH maintained at 5) on the polishing of silicon dioxide and silicon nitride. The promoting or inhibitory effects of amino acids first increased and then decreased with increasing concentration. When 0.02 M lysine and 0.02 M glutamic acid were added to 0.5 wt% CeO2 dispersion, the best effect was achieved. At this time, the material removal rate (MRR) of SiO2 and Si3N4 were 2993.4 Å/min and 137.2 Å/min, respectively, with surface roughness of 0.108 nm and 0.142 nm in the 5 μm × 5 μm region. This study shows that amino acids promote the MRR of SiO2 primarily by enhancing the reactivity of Ce4+ by complexing with carboxyl groups. In contrast, amino acids inhibit the MRR of Si3N4 primarily by forming strong hydrogen bonds between the amino group and its surface, resulting in surface adsorption and suppressing the hydrolysis reaction. The CMP mechanisms of the three amino acids are similar, and the differences in their effects are mainly due to the varying numbers of amino and carboxyl groups they carry. The adsorption of three amino acids on SiO2 and Si3N4 surfaces was simulated by Materials Studio software, and the results were consistent with the experimental results. Finally, this paper explained the mechanism of action of amino acids at the microscopic level and provided some guidance on improving the performance of CeO2 slurry.