The present article reports on a strategy for the functionalization of multi‐walled carbon nanotubes (MWCNTs) by grafting with various polymer chains. Copolymers consisting of α‐methylstyrene (AMS) and a second monomer, that is glycidyl methacrylate (GMA) or styrene (St), were synthesized in advance. The copolymers were heated in the presence of MWCNTs in solution, decomposition of the AMS sequences occurred, providing macroradicals, which further attacked the double bonds on the MWCNT surfaces. Grafting of the copolymer chains onto the surface of the MWCNTs was thus achieved, as demonstrated by FT‐IR, XPS and Raman technologies. The resulting poly(AMS‐co‐GMA)‐g‐MWCNTs could be uniformly dispersed in N,N‐dimethylformamide (DMF) and acetone, and the poly(AMS‐co‐St)‐g‐MWCNTs also could be uniformly dispersed in DMF.
