To enhance the performance of cerium oxide polishing slurry and improve the polishing efficiency of Nd-glass without destroying the surface quality of Nd-glass, anionic surfactant Lamepon A was chosen to be added to the cerium oxide polishing slurry. In this work, the effects of the modified polishing slurry on the particle size of the cerium oxide polishing slurry, material removal rate of Nd-glass, and surface quality of Nd-glass after polishing were studied. The effect of pH of polishing slurry with different mass fraction of Lamepon A on the polishing rate and quality of Nd-glass were also studied. The results show that Lamepon A can inhibit the agglomeration of nanoparticles in the polishing slurry, reduce the median diameter of cerium oxide, and improve the polishing efficiency. When the mass fraction of the cerium oxide is 3%, the pH is 6.5, and mass fraction of Lamepon A is 0.30%, the material removal rate attains a maximum value of 169 nm/min; when the mass fraction of the cerium oxide is 3%, the pH is 7, the mass fraction of Lamepon A is 0.20%, the surface roughness reaches a minimum of 0.9 nm.