In this study, carbon nanotube-based adsorbents, oxidized multi-walled carbon nanotube (OMWCNT) with non-magnetic property and OMWCNT-Fe3O4 and OMWCNT-κ-carrageenan-Fe3O4 nanocomposites with magnetic property, having different structural and surface properties were prepared and their adsorptive properties for the removal of toxic diquat dibromide (DQ) herbicide from water by adsorption were determined in detail. For each adsorption system, the effects of initial DQ concentration, contact time and temperature on the adsorption processes were determined. Equilibrium time was found to be 300 min for DQ solutions. OMWCNT showed faster adsorption and higher maximum adsorption capacity value than magnetic adsorbents. With increasing initial herbicide concentration from 5.43 mg.L−1 to 16.3 mg.L−1, the values of initial sorption rate exhibited a decrease from 29.1 mg.g−1.min−1 to 4.28 mg.g−1.min−1 for OMWCNT-DQ system, from 1.21 mg.g−1.min−1 to 0.823 mg.g−1.min−1 for OMWCNT-Fe3O4-DQ system and from 0.674 mg.g−1.min−1 to 0.612 mg.g−1.min−1 OMWCNT-κ-carrageenan-Fe3O4 system. Maximum adsorption capacity value of OMWCNT was approximately 2.8-fold higher than magnetic OMWCNT-Fe3O4 and 5.4-fold higher than magnetic OMWCNT-κ-carrageenan-Fe3O4 at 25 °C. Adsorption kinetic and isotherm data obtained for all adsorption systems were well-fitted by pseudo second-order and Langmuir models, respectively. Thermodynamic parameters indicated that the adsorption of DQ onto carbon nanotube-based adsorbents was spontaneous and endothermic process. Furthermore, OMWCNT having the highest herbicide adsorption capacity could be regenerated and reused at least five times. This study showed that carbon nanotube-based adsorbents with magnetic and non-magnetic property were of high adsorption performance for the removal of DQ from water and could be promising adsorbent materials for the efficient removal of herbicides from wastewaters.