Antimony (Sb) is one of the most concerning toxic metals globally, making the study of methods for efficiently removing Sb(III) from water increasingly urgent. This study uses graphene oxide and chitosan as the matrix (GOCS), modifying them with FeCl2 and four MnOx to form iron-manganese oxide (FM/GC) at a Fe/Mn molar ratio of 4:1. FM/GC quaternary composite microspheres are prepared, showing that FM/GC obtained from different MnOx exhibits significant differences in the ability to remove Sb(III) from neutral solutions. The order of Sb(III) removal effectiveness is MnSO4 > KMnO4 > MnCl2 > MnO2. The composite microspheres obtained by modifying GOCS with FeCl2 and MnSO4 are selected for further batch experiments and characterization tests to analyze the factors and mechanisms influencing Sb(III) removal. The results show that the adsorption capacity of Sb(III) decreases with increasing pH and solid-liquid ratio, and gradually increases with the initial concentration and reaction time. The Langmuir model fitting indicates that the maximum adsorption capacity of Sb(III) is 178.89 mg/g. The adsorption mechanism involves the oxidation of the Mn-O group, which converts Sb(III) in water into Sb(V). This is followed by ligand exchange and complex formation with O-H in FeO(OH) groups, and further interactions with C-OH, C-O, O-H, and other functional groups in GOCS.