Inherent shortcomings including low hardness and poor wear-resistance have become the important factors limiting the industrial application of polymer materials in some harsh environments. In order to improve the surface hardness and wear-resistance, various surface modification techniques have been applied to the wear protection of polymer materials. Among these surface modifications, fabricating a layer of amorphous carbon-based coating is one of the greatest potential approaches to improve the surface hardness and wear-resistance of polymer materials. The research progress of amorphous carbon-based coatings for improving the wear-resistance of polymer materials was reviewed, and the essential reason of poor adhesive strength of amorphous carbon-based coatings on the surface of polymer materials was analyzed. The mismatch between polymer materials and amorphous carbon coatings in structures and properties made the abrupt interface unstable under loading, resulting in the poor adhesive strength. Various methods commonly used to improve the adhesive strength of amorphous carbon coatings on polymer materials were discussed and compared. The reliable adhesive strength of amorphous carbon coatings could be obtained by the plasma treatment on the surface of polymer materials, which could induce a gradual transformation from organic carbonaceous structures into inorganic carbonaceous structures. An in-situ transition layer could be constructed on the polymer substrates by plasma treatment. The in-situ transition layer provided reliable adhesive strength between amorphous carbon coatings and polymer substrates via chemical bond, which endowed an effective improvement of the hardness, anti-friction and wear-resistance of polymer materials.