In order to explore the effect of –OH functional groups in Cs⁺ adsorption, we herein used the low temperature plasma-induced grafting method to graft chitosan onto carbon nanotubes (denoted as CTS-g-CNTs), as raw-CNTs have few functional groups and chitosan has a large number of –OH functional groups. The synthesized CTS-g-CNT composites were characterized using different techniques. The effect of –OH functional groups in the Cs⁺ adsorption process was evaluated by comparison of the adsorption properties of raw-CNTs with and without grafting chitosan. The variation of environmental conditions such as pH and contact time was investigated. A comparison of contaminated seawater and simulated groundwater was also evaluated. The results indicated that: (1) the adsorption of Cs⁺ ions was strongly dependent on pH and the competitive cations; (2) for CNT-based material, the –OH functional groups have a positive effect on Cs⁺ removal; (3) simulated contaminated groundwater can be used to model contaminated seawater to evaluate the adsorption property of CNTs-based material. These results showed direct observational evidence on the effect of –OH functional groups for Cs⁺ adsorption. Our findings are important in providing future directions to design and to choose effective material to remedy the removal of radioactive cesium from contaminated groundwater and seawater, crucial for public health and the human social environment.