The present study deals with the preparation of nanomagnetite (NM), potassium carrageenan (KC), and nanomagnetite/potassium carrageenan bio-composite beads (NC). Characterization of the prepared solid materials using different physicochemical techniques such as X-ray diffraction analysis (XRD), thermogravimetric analysis (TGA), scanning electron microscopy (SEM), transmission electron microscope (TEM), energy-disperse X-ray spectroscopy (EDX), diffuse reflectance spectrophotometer (DRS), swelling ratio (SR%), N2 adsorption, pH of point of zero charges (pHPZC), and Fourier transform infrared spectroscopy (FTIR). Comparing between adsorption and photo-Fenton degradation process for methylene blue (MB) on the surface of the prepared solid materials. Nanomagnetite/potassium carrageenan bio-composite (NC) exhibited high specific surface area (406 m2/g), mesoporosity (pore radius, 3.64 nm), point of zero charge around pH6.0, and the occurrence of abundant oxygen-containing functional groups. Comparison between adsorption and photo-Fenton oxidation process for methylene blue (MB) was carried out under different application conditions. NC exhibited the maximum adsorption capacity with 374.50 mg/g at 40 °C after 24 h of shaking time while 96.9% of MB was completely degraded after 20 min of photo-Fenton process. Langmuir's adsorption model for MB onto the investigated solid materials is the best-fitted adsorption model based on the higher correlation coefficient values (0.9771–0.9999). Kinetic and thermodynamic measurements prove that adsorption follows PSO, endothermic, and spontaneous process, while photo-Fenton degradation of MB achieves PFO, nonspontaneous, and endothermic process. Photo-Fenton degradation is a fast and simple technique at a lower concentration of dye (< 40 mg/L) while at higher dye concentration, the adsorption process is preferred in the removal of that dye.