This paper reports a high efficiency uptake of captopril (CPT), employing magnetic graphene oxide (MGO) as the adsorbent. The graphene oxide (GO) was produced through an oxidation and exfoliation method, and the magnetization technique by the co-precipitation method. The nanomaterials were characterized by FTIR, XRD, SEM, Raman, and VSM analysis. The optimal condition was reached by employing GO·Fe3O4 at pH 3.0 (50 mg of adsorbent and 50 mg L−1 of CPT), presenting values of removal percentage and maximum adsorption capacity of 99.43% and 100.41 mg g−1, respectively. The CPT adsorption was dependent on adsorbent dosage, initial concentration of adsorbate, pH, and ionic strength. Sips and Elovich models showed the best adjustment for experimental data, suggesting that adsorption occurs in a heterogeneous surface. Thermodynamic parameters reveal a favorable, exothermic, involving a chemisorption process. The magnetic carbon nanomaterial exhibited a high efficiency after five adsorption/desorption cycles. Finally, the GO·Fe3O4 showed an excellent performance in CPT removal, allowing future application in waste management.