A bimetallic organic gel (MOG-Fe/Al) was synthesized through the solvothermal method. The gel state of the product obtained under optimized gel formation conditions is sufficient to carry 2 g of weight for a long time. Scanning electron microscopy (SEM), X-ray diffraction (XRD), Fourier transform infrared (FT-IR) spectroscopy, Brunauer–Emmett–Teller (BET) technique, and X-ray photoelectron spectroscopy (XPS) analysis confirmed the structures and morphologies of the synthesized materials. MOG-Fe/Al, with good stability, excellent durability, and wide applicability, exhibited efficient MO adsorption capacity as high as 335.88 mg/g at 25 °C. Adsorption-influencing factors including solution pH, contact time, and temperature were investigated. The adsorption performance of the bimetallic organic gel was better than that of the monometallic organic gels (MOG-Fe and MOG-Al), and its adsorption processes were in accordance with the pseudo-second-order kinetic and Langmuir isothermal models. The excellent adsorption capacity of the MOG-Fe/Al is due to its surface structure, pore volume, π-π interactions, hydrogen bonds, and electrostatic interactions.