In this work, FeS was anchored on mesoporous silica microspheres (SiO2200, SiO2500, and SiO21000), and named as FeS@SiO2 (i.e., FeS@SiO2200, FeS@SiO2500, FeS@SiO21000), in adsorbing and detoxifying U(VI)/Cr(VI) from wastewater. Results demonstrated that FeS@SiO2 exhibited higher efficiency towards U(VI)/Cr(VI), outperforming FeS and SiO2 alone. Kinetic investigations revealed that adsorption of U(VI)/Cr(VI) followed pseudo–second–order model best, highlighting effective chemical interplay. XPS investigations demonstrated multi–species which was included FeS, Fe(II), S2− and polysulfide (S22−, Sn2−) could be employed as reductants for U(VI)/Cr(VI) adsorption. The combination of SiO2 and FeS offered an enhanced efficiency for U(VI)/Cr(VI), making these composites promising materials in water purification.