Currently reported adsorbents for wastewater purification generally have only limited adsorption capacity and low adsorption rate towards dye contaminants. In this work, KH570-modified magnetic hydrogel nanocomposites (KH570-mHNCs) with semi-IPNs structure were prepared based on poly (acrylamide-co-acrylic acid), polyvinyl pyrrolidone (PVP), and KH570-modified magnetic nanoparticles, and it exhibited high absorption capacity and absorption rate for methylene blue dye. KH570-mHNCs had a rough surface with many porous and gully structures, and FTIR results preliminarily confirmed the target structure of KH570-mHNCs. KH570-mHNCs could rapidly absorb methylene blue by approaching absorption equilibrium at 90 min. Dye absorption of KH570-mHNCs had maximum dye absorption capacity at pH = 8, and methylene blue adsorption capacity was 255.4 mg/g, 326.3 mg/g, and 418.5 mg/g in the condition of initial dye concentrations of 700 mg/L, 900 mg/L, and 1100 mg/L, respectively. Methylene blue adsorption isotherms and kinetics conformed to the Langmuir model and pseudo-second-order kinetic model, respectively. Methylene blue adsorption for KH570-mHNCs was a spontaneous, exothermal, and entropy reduction process. In addition, KH570-mHNCs had good magnetic response, desorption, and reusability, which made it a potential application in the field of methylene blue removal from the aqueous solution.