Composites comprised of chitosan (CS) and multiwalled carbon nanotubes (MWCNTs) were fabricated by milling and ultrasonication dispersion methods. Scanning electron microscopy images showed homogeneous dispersion of MWCNTs throughout the CS matrix for samples prepared by either ultrasonication or milling methods. Further, the crystallinity of the CS component was found to decrease with the addition of MWCNTs, although the decomposition temperature and the storage modulus (E′) of the samples were improved. The decomposition temperature for the composite prepared by milling was 7°C higher than that by the ultrasonication. Meanwhile, the E′ decreased relatively slowly with temperature in the dynamic mechanical analysis measurements. In addition, IR analysis implied an interaction between CS and MWCNTs, which likely originated from hydrogen bonds between the amino, hydroxyl, and carboxyl groups of the two components. Compared with the ultrasonication, milling was more effective to promote the formation of the hydrogen bonds between CS and the MWCNTs and thus enhance the thermal stability of CS.