It is well known that pure polymeric materials by themselves cannot be used for high-performance applications in every field owing to their inadequate properties. In addition, the modification of substrate surfaces is essential for numerous applications.[1] A polymer brush is an assembly of polymer chains that are tethered at one end to a surface or an interface.[2] The grafting of polymer brushes on a substrate surface provides a practical tool for surface modification and functionalization. With the aim of not influencing the mechanical properties of a given substrate, the modification of the substrate with grafted polymer brushes can significantly affect the surface properties, such as friction, adhesion, wettability, and biocompatibility.[3] Furthermore, the real importance of such a modification is that it provides a method to enhance the surface properties while maintaining the original matrix performance. However, the method of grafting polymer brushes still faces some obstacles; for example, poor robustness has become a bottleneck for large-scale biomedical, industrial, or clinical applications of the modified surfaces. At present, surface modification methods of polymeric substrates can be divided into physical and chemical methods.