Structure-designed free-standing diamond films have been fabricated by DC plasma jet method. The different dominant crystalline surface distributions were obtained under different deposition conditions. The as-grown films were polished by thermal chemical method. For the same crystalline structure, the removal rate was strongly affected by polishing parameters, such as polishing temperature, polishing time and applied pressure. The experimental results also showed that the dominant surface distribution in the films affected the polishing removal rate very much.