Novel quaternary ammonium/magnetic graphene oxide composites (M-PAS-GO) that efficiently remove Cr(VI) ions were fabricated through the introduction of the (3-aminopropyl) triethoxysilane and Fe3O4 nanoparticles on the surface of GO, and then modified with n-butyl bromide. The fabricated M-PAS-GO was comprehensively characterized by SEM, TEM, EDX, XRD, Raman spectroscopy and FTIR, and the results manifest that the quaternary ammonium group was introduced onto the surface of GO. Under the reaction conditions of pH 3.20, temperature of 25 °C and M-PAS-GO dosage of 0.01 g/50 mL, 90% of 10 mg/L Cr(VI) ions were removed from the solution within 20 min. The kinetics study indicates that the adsorption process followed the pseudo-second-order model and was surface reaction-controlled. The thermodynamic parameters calculated from temperature-dependent adsorption isotherms suggest that the adsorption process was an exothermic and spontaneous process. The maximum adsorption capacities of Cr(VI) ions on M-PAS-GO composites calculated by the Langmuir model were 46.48 mg/g. Moreover, the reusability and stability of M-PAS-GO demonstrates its economic sustainability. This study suggests that M-PAS-GO is a potential candidate adsorbent for the separation of Cr(VI) from wastewater.