Glow discharge polymer (GDP) capsules are often used as the ablation layer in laser inertial confinement fusion (ICF) research, because of its excellent properties in low X-ray opacity, high tensile strength, and high thermal conductivity. The isolated surface defects and distribution of oxygen content on the surface of GDP capsules can lead to the increase of hydrodynamic instability and the decrease of compression efficiency. In this work, by using media spheres and silica nanoparticles, a tumble polishing device for GDP capsule polishing is built to improve the surface morphology. The effects of polishing parameters on the surface roughness and oxygen content of GDP were investigated. The test results show that tumble polishing can effectively remove convex defects, only 24 identified defects with a height below 231 nm were found after 144 h polishing, reduce the surface roughness (∼10 nm) and improve the surface quality of GDP capsules. Moreover, the oxygen content distribution on the surface of GDP is uniform after tumble polishing. And the depth analysis results show that the tumble polishing has no obvious effect on the change of oxygen content in GDP shell under the surface layer.