Corona discharge treatment at atmospheric pressure was applied to initiate the graft polymerization of 2‐hydroxyethyl methacrylate onto the surface of multi‐walled carbon nanotubes (MWCNTs). The results indicated that MWCNTs were encapsulated by poly(2‐hydroxyethyl methacrylate) (PHEMA). The blue shift and the increased ID/IG value of the Raman spectra confirmed the covalent attachment of PHEMA onto the surface of the MWCNTs. The grafting degree depended on the processing time of corona discharge, as demonstrated by thermogravimetric analysis. The dispersibility of the PHEMA grafted MWCNTs (PHEMA‐g‐CNTs) in ethanol was dramatically improved. It was also found that PHEMA‐g‐CNTs can improve the dynamic mechanical and mechanical properties of the nanocomposites more effectively than the pristine MWCNTs.