Water-soluble hyperbranched polyamine functionalized multiwalled carbon nanotubes nanocomposite (WHPA-OMCNT) was successfully prepared and applied to water remediation in this paper. WHPA-OMCNT was characterized by Fourier transform infrared spectroscopy (FTIR), thermogravimetric analysis (TGA), zeta potential, scanning electron microscopy (SEM) and transmission electron microscope (TEM) analyses. WHPA-OMCNT exhibited excellent adsorption performance for removal of organic dyes e.g., methylene blue (MB), malachite green (MG) and methyl violet (MV). The equilibrium adsorption capacity was 800.0 mg g-1 for MB, 840.3 mg g-1 for MG and 970.9 mg g-1 for MV under the optimal conditions. The pseudo-second order equation and the Langmuir model exhibited good correlation with the adsorption kinetic and isotherm data for all three pollutants, respectively. The thermodynamic results (ΔG < 0, ΔH < 0, ΔS < 0) implied that the adsorption process of MB, MG and MV was feasible, exothermic and spontaneous in nature. A possible adsorption mechanism has been proposed, where H-bonding, electrostatic attraction and π-π stacking interactions dominated the adsorption of the organic dyes. In addition, the excellent reproducibility endowed WHPA-OMCNT with the potential for application in water treatment.