Methylene blue (MB) is one of the toxic synthetic dyes that are being discharged heavily into water supplies. Hence, MB removal is one of the most important tasks for a cleaner water supply. By using inexpensive, abundant, and easy-to-synthesize materials, superparamagnetic iron oxide nanoparticles, which were synthesized using the co-precipitation method with polyvinyl alcohol and graphite (SPION/PVA/GR), can be used to adsorb MB. The adsorbent was characterized using FE-SEM, FTIR, XRD, VSM, and BJH. The entrapment efficiency of MB on SPION/PVA/GR after 12 days was 33.96 ± 0.37–42.55 ± 0.39%, at 333.15, 310.15, and 298.15 K, and the initial concentration of MB was 0.017–0.020 mg/mL. The adsorption process can be considered spontaneous, endothermic, chemisorption, heterogeneous, or multilayer adsorption. When releasing MB at 298.15 K and a pH of 3.85 after 7 days, the release percentage ranged from 11.56 ± 0.33 to 22.93 ± 5.06 depending on the initial loading conditions and mainly the releasing temperature following the Higuchi kinetic model. Since this is a novel SPION-based MB adsorbent, optimization, and different forms of adsorbent (i.e., thin film composite) should be further researched.