The aggregates of carbon nanotubes in aqueous solution limit their potential application as effective adsorbents for organic contaminants. In the present study, Manganese dioxide coated on multi-walled carbon nanotubes (MnO2/MWNT) was prepared by redox reaction. Adsorption properties of two dyes (malachite green and rhodamine B) on MnO2/MWNT were examined to explore the potential of MnO2/MWNT for the removal of dyes from aqueous solutions. Compared with MWNT, MnO2/MWNT showed extraordinarily high adsorption affinity for both tested dyes, adsorption of the test dyes was enhanced 3-10 times. It was proposed that the strong adsorption mechanisms were π−π electron donor-acceptor interaction and Lewis acid-base interaction. The effecst of pH and dissolved humic acids on adsorption were also assessed. For two dyes, similar patterns of pH-dependent adsorption were observed, implying the predominance of graphene structures for the adsorption to MnO2/MWNT. The presence of humic acids suppressed the adsorption of two dyes on MnO2/MWNT.