Removal of lead ions from drinking water is one of the biggest global issues. In this study, green modification of multi-walled carbon nanotubes (MWCNTs) was performed by calcium ferrite (CNT@CaF) and magnesium ferrite (CNT@MgF). Taxus wallichiana (T.W) was used as green template. For comparison, bare CNTs were also studied to evaluate the effect of surface functionalization. The morphology, composition, functional groups analysis, surface area and charge characteristics were performed by Transmission Electron Microscopy (TEM), X-ray Diffraction (XRD), Fourier-Transform Infrared Spectroscopy (FTIR), Energy-Dispersive X-ray Spectroscopy (EDX), Barrett-Joyner-Halenda (BJH), Point of Zero Charge (PZC) and zeta potential. BET surface area of CNTs, CNT@CaF and CNT@MgF calculated as 98 m2/g, 186 m2/g, and 206 m2/g respectively. The adsorption behavior of Pb2+ ion was determined under the influence of contact time, pH, temperature, concentration, and dose. The results manifested that functionalized adsorbents showed incredible removal efficiency of Pb2+ ions (81–85%). Langmuir and Pseudo second order (PSO) models were found suitable for data fitting. The maximum adsorption capacities of 58.5 mg/g, 371.7 mg/g, and 210.9 mg/g were calculated for CNTs, CNT@CaF and CNT@MgF respectively. Separation factor (RL) values further supports the favorable sorption on the sorbent’s surface. The desorption and thermodynamic studies support chemisorption as a dominating mechanism. However, spectroscopic studies revealed the mixed sorption mechanisms i.e., inner sphere complexation and electrostatic interactions are simultaneously taking place.