In this study, composite hydrogels were prepared using a simple synthetic technique to adsorb methylene blue (MB) from water. The hydrogel comprised potassium persulfate (KPS) as the initiator, N,N′-methylene bisacrylamide as the crosslinking agent, and sodium hydroxide (NaOH) as the activator. It was employed to adsorb MB at different concentrations from water. The morphology and properties of PUL/PAM/GO composites were characterized through thermogravimetric analysis, Fourier transform infrared spectroscopy, and scanning electron microscopy. Moreover, the adsorption properties, adsorption isotherms, adsorption kinetics, adsorption thermodynamics, and swelling properties of the hydrogel for MB were investigated. The optimal ratio of PUL to AC was obtained as 6:1 by fixing the amount of PUL and loading AC of different masses. The maximum adsorption capacity was obtained as 591.4 mg/g. It also exhibited certain mechanical strength. The adsorption of MB conforms to pseudo-first-order kinetics and Langmuir isotherms. In this study, an environment-friendly, cheap, simple, and efficient way was presented for the composite hydrogel in the direction of water treatment.