A simple and facile method for the non-covalent functionalization of multi-walled carbon nanotubes (MWNTs) using poly(4-styrenesulfonic acid) (PSS) is proposed. The resulting PSS-MWNTs dispersion is readily soluble in water and can be left to stand for 2 weeks at room temperature, no phase separation with aggregation of nanotubes at the bottom of the vials was observed. The as-prepared PSS-MWNTs dispersions could facilitate the processing of the nanotubes into composites with high nanotube loading. The PSS-MWNTs complex shows high electrocatalytic activity to the oxidation of neutrontransmitter of dopamine, suggesting that the coating of PSS onto carbon nanotubes surface without destroying the electronic structures of the pristine carbon nanotubes; therefore, the unique properties including the catalytic property of the nanotubes retained. It is envisioned that the PSS-MWNTs aqueous dispersions may find possible applications in the development of biosensors, bioelectronics, separation and environment protection as well as other biological events where water-based environment is required.