The nanocomposites XFe₂O₄/GO with various metal sites (X = Co, Mn, and Ni) were successfully synthesized via the polymerized complex method. The XFe₂O₄/GO family was characterized using X-Ray diffraction analysis, scanning electron microscopy (SEM), and a vibrating sample magnetometer. We also investigated the effect of three fundamental parameters (initial concentration, dosage, and pH) on the removal of methylene blue using the response surface methodology. A high F value, very low P value (< 0.00001), a non-significant lack of fit, and the determination coefficient (R ² > 0.95) demonstrated a strong correlation between experimental and predicted values of the responses. The predicted optimal conditions for maximum removal efficiency were easily determined to adhere to the following trend for actual test experiments: MnFe₂O₄/GO (60.1%) < CoFe₂O₄/GO (80.3%) < NiFe₂O₄/GO (87.7%). Moreover, the adsorption behavior was well-described by the Langmuir isotherm and a pseudo-second-order kinetic model. The maximum capacity for adsorption of methylene blue onto XFe₂O₄/GO was found from 42.2 to 80.6 mg/g. Moreover, the XFe₂O₄/GO could be regenerated for several cycles without a considerable decrease in removal yield, suggesting that this highly promising XFe₂O₄/GO could be applied as an efficient and novel adsorbent.