The manuscript presents the results on the sorption of U(VI), Am(III) & Eu(III) from pH medium by anovel amido-amine functionalized multiwalled carbon nanotube (MWCNT). The novel functional groupwas introduced in the MWCNT by two step processes and characterized by various instrumental tech-niques like Scanning Electron Microscopy (SEM), Raman and X-ray Photoelectron Spectroscopy (XPS).The sorption process was found to be highly dependent on the pH of the solution with maximum sorptionfor both 233U, 241Am & 152+154Eu at pH 7.0. Kinetics of sorption was found to be fast with equilibriumreached in ∼15 min and the sorption was found to be following pseudo 2nd order kinetics for the radionu-clides. The sorption for both 233U and 152+154Eu followed Langmuir sorption model with maximumsorption capacity of 20.66 mg/g and 16.1 mg/g respectively. This has been explained by DFT calculationswhich shows that more negative solvation energy of U(VI) compared to Am(III) and Eu(III) and strongerU-MWCNT-AA complex is responsible for higher sorption capacity of U(VI) compared to Am(III) andEu(III).The synthesized amido-amine functionalized MWCNT is a very promising candidate for removalof actinides and lanthanides from waste water solution with high efficiency