This work focused on evaluating the adsorptive removal of crude oil using a nano-intermediate based on magnetite nanoparticles supported on activated carbon synthesized from spent coffee grounds and the subsequent catalytic oil decomposition to recover by-products and regenerate the support material. The magnetite nanoparticles were synthesized by the co-precipitation method and were used as active phases on prepared activated carbon. The amount of crude oil adsorbed was determined by adsorption isotherms. In addition, dynamic tests were performed on a packed bed to evaluate the efficiency of the removal process. Thermogravimetric analysis and mass spectrometry were used to evaluate the catalytic powder and the quantification of by-products. Contrasting the results with commercial carbon, the one synthesized from the coffee residue showed a greater affinity for the oil. Likewise, the adsorption capacity increased by doping activated carbon with magnetite nanoparticles, obtaining an efficiency greater than 10%. The crude oil decomposition was carried out successfully by thermal cracking, obtaining a 100% removal. The gas produced after decomposition contains light hydrocarbons such as C2H4 and CH4 and shows a decrease in polluting species such as CO and CO2, leading to greater environmental sustainability of the process.