New hydrogels (HG) were synthesized in aqueous medium by free radical polymerization of N,N-dimethylacrylamide (DMAA) and 2-oxazoline macromonomer (MM) initiated by potassium persulfate (KPS) and catalyzed by N,N,N,N′-tetramethylethylenediamine (TEMED). In this polymerization, the monomer DMAA was also used as a crosslinker because it has the ability of self-crosslinking in the presence of peroxodisulfate initiator type. The macromonomer (DP = 24) was a gradient copolymer of 2-methyl-2-oxazoline and methyl-3-(oxazol-2-yl)-propionate with a styryl end group. 1H high-resolution (HR)-MAS NMR spectroscopy allowed to confirm the structure of hydrogels and to determine the molar content of DMAA and MM in each of them. Hydrogels (HG-H) containing carboxylic groups were obtained by basic hydrolysis of HG. Hydrolyzed hydrogels (HG-H) were used for the adsorption of methylene blue (MB) in aqueous medium. It was found that the MB adsorption increased as the initial MB concentration increased, and maximum adsorption capacities were found. The influence of pH value on MB adsorption was evaluated, showing that the MB adsorption capacity of the hydrogels was higher at pH value ≥ 5.7. Adsorption isotherms were studied using Langmuir and Freundlich models. The latter model describes best the process suggesting a possible adsorption mechanism through electrostatic interactions between MB and HG-H hydrogels. The MB adsorbed inside the hydrogels, could be removed with an acidic solution and therefore the hydrogel could be applied to adsorb MB again.