Lignocellulose (LNC) multi-walled carbon nanotubes (MWCNTs) composites were synthesized by covalently grafting a natural polymer, lignocellulose, onto MWCNTs in an ionic liquid, 1-allyl-3-methylimidazolium chloride (AmimCl). Furthermore, the grafting of LNC facilitated the dispersion of the MWCNTs in AmimCl and MWCNTs/LNC films. The elongation at break and tensile strength of grafted-MWCNTs/LNC films with 3wt% of MWCNTs content were 12.2% and 106.7MPa respectively, which was almost 93.7% and 10.7% higher than those of the pristine MWCNTs/LNC films. This finding clearly revealed that the mechanical properties of grafted-MWCNTs/LNC films were dramatically superior to those of the MWCNTs/LNC films.