In this work, stabilized ionotropic hydrogels were designed using sodium carboxymethyl cellulose (CMC) and assessed as inexpensive sorbents for hazardous chemicals (e.g., Methylene Blue, MB) from contaminated wastewaters. In order to increase the adsorption capacity of the hydrogelated matrix and facilitate its magnetic separation from aqueous solutions, sodium dodecyl sulfate (SDS) and manganese ferrite (MnFe2O4) were introduced into the polymer framework. The morphological, structural, elemental, and magnetic properties of the adsorbents (in the form of beads) were assessed using scanning electron microscopy (SEM), energy-dispersive X-ray analysis, Fourier-transform infrared spectroscopy (FTIR), and a vibrating-sample magnetometer (VSM). The magnetic beads with the best adsorption performance were subjected to kinetic and isotherm studies. The PFO model best describes the adsorption kinetics. A homogeneous monolayer adsorption system was predicted by the Langmuir isotherm model, registering a maximum adsorption capacity of 234 mg/g at 300 K. The calculated thermodynamic parameter values indicated that the investigated adsorption processes were both spontaneous (ΔG< 0) and exothermic (ΔH< 0). The used sorbent can be recovered after immersion in acetone (93% desorption efficiency) and re-used for MB adsorption. In addition, the molecular docking simulations disclosed aspects of the mechanism of intermolecular interaction between CMC and MB by detailing the contributions of the van der Waals (physical) and Coulomb (electrostatic) forces.