Ballonet polishing is a new type of flexible polishing technology in the optical polishing. The polishing experiment is implemented on the flexible ballonet polishing device. Three kinds of different polishing layer materials are used in the experiment. Surface roughness and surface defect of the samples of these layer materials are analyzed. The experimental results show that the woolen cloth is a good layer material which can get high processing efficiency, while the velvet material gets low surface defect on polishing sample.