Multi-walled carbon nanotubes (MWCNTs) have displayed great potential as catalyst carriers due to their nanoscale structure and large specific surface area. However, their hydrophobicity and poor dispersibility in water restrict their applications in aqueous environments. Herein, the dispersibility of MWCNTs was significantly enhanced with a chimeric protein MPKE which consisted of a zwitterionic peptide unit and a mussel adhesive protein unit. The MPKE could be easily attached to MWCNTs (MPKE-MWCNTs) by a simple stirring process due to the versatile adhesion ability of mussel adhesive unit. As expected, the MPKE-MWCNTs displayed outstanding dispersibility in water (>7 months), as well as in alkaline solutions (pH = 12) and organic solvents (DMSO and ethanol) due to the hydrophilicity of the zwitterionic peptide unit. Moreover, the MPKE-MWCNTs were used as silver nanoparticle carriers for the reduction of 4-nitrophenol in wastewater, with the normalized rate constant k_nor up to 32.9 s⁻¹ mmol⁻¹. Meanwhile, they also exhibited excellent biocompatibility and antibacterial activity, which were favorable for wastewater treatment. This work provides a facile strategy for MWCNT modification, functionalization and applications in aqueous environments.