The removal of Ni2+ from aqueous solution by magnetic multiwalled carbon nanotube nanocomposite (MMWCNTs-C) was investigated. MMWCNTs-C was characterized by X-ray Diffraction method (XRD), High-Resolution Transmission Electron Microscopy (HRTEM), surface area (BET), and Fourier Transform-Infrared Spectroscopy (FTIR). The effects of initial concentration, contact time, solution pH, and temperature on the Ni2+ adsorption onto MMWCNTs-C were studied. The Langmuir and Freundlich isotherm models were applied to fit the adsorption data. The results showed that the adsorption isotherm data were fitted well to the Langmuir isotherm model with the maximum monolayer adsorption capacity of 2.11 mg g–1. The adsorption kinetics was best described by the pseudo-second-order model. The thermodynamic parameters, such as ΔHo, ΔGo and ΔSo, were also determined and evaluated. The adsorption of Ni2+ is generally spontaneous and thermodynamically favorable. The values of ΔHo and ΔGo indicate that the adsorption of Ni2+ onto MMWCNTs-C was a physisorption process.