Poly(2-diethylaminoethyl methacrylate) (PDEAEMA)-coated multiwalled carbon nanotubes (MWNT- PDEAEMA) were successfully prepared by MWNT-surface initiated atom transfer radical polymerization (ATRP). The obtained MWNT-PDEAEMA nanocylinders have a core of MWNT and a shell of PDEAEMA and this core-shell structure was confirmed by TEM observations. The UV-Vis and AFM measurements showed that the MWNT-PDEAEMA exhibited obvious pH sensitivity. The solubility of PDEAEMA-coated MWNT dramatically decreased when pH increased to ca. 7.0. Because of the giant molecular weight of the molecular hybrids and local high density of polymeric grafts linked onto MWNTs, the resulting MWNT-PDEAEMA nanocomposites are easier to aggregate, or more sensitive to pH, as compared with the neat PDEAEMA.