Gemini surfactant/GO composites (10-2-10/GO, 12-2-12/GO, and 14-2-14/GO) have been successfully prepared using three gemini surfactants with different tail chain lengths. The morphology and physicochemical properties of the as-synthesized composites were characterized by scanning electron microscopy, transmission electron microscopy, Fourier transform-infrared spectroscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. The gemini surfactant/GO composites were applied to the adsorption of Congo red dye, and from the experimental data, optimum adsorption conditions, adsorption kinetics, and isotherms were obtained. The removal process was favorable at acidic pH and reached equilibrium in ∼60 min. The results showed that the pseudo-second-order model and the Langmuir adsorption isotherm were a good fit for the adsorption of Congo red onto gemini surfactant/GO composites. Compared with other adsorbents reported in the literature, these composites showed superior Congo red adsorption capabilities, with absorption capacities as high as 2116, 2193, and 2325 mg g for 10-2-10/GO, 12-2-12/GO, and 14-2-14/GO, respectively. Moreover, the adsorption capacities were more than 1000 mg g even for the fifth cycle. The results of the present study substantiate that the gemini surfactant/GO composites are promising adsorbents for the removal of organic dyes in wastewater treatment.