Sustainable development has become an inevitable trend in the world's green chemical industry for a generation or more. In this study, a monodisperse magnetic polystyrene mesoporous composite microsphere (MPPS) composed of Fe3O4 nanoparticles loaded on polystyrene mesoporous microspheres is introduced. These microspheres serve as effective adsorbents for the swift removal of cationic dyes. The fabrication of the wastewater adsorbent, with its simple operation and economic practicality, involved a combination of dispersion polymerization, a sulfonation reaction, two-step swelling polymerization, and in situ alkaline oxidation technology. Notably, the adsorption capacity within 3 min reaches 184.0 mg/g, with an impressive adsorption efficiency of 92%. This is primarily attributed to the high specific surface area (Smax) of the MPPS providing more reaction sites for π-π interaction. Simultaneously, the attractive force between negatively charged sulfonic acid groups and cationic dyes is enhanced through surface modification of the MPPS. Furthermore, the MPPS, boasting a maximum saturation magnetization of 38.19 emu/g, ensures rapid separation from the solution for recycling within 3 s. Even after 5 cycles, the adsorption efficiency remains over 90%. The rapid separation of dyes is facilitated by the magnetic attraction of Fe3O4 nanoparticles from the MPPS under the application of a magnetic field. These composite mesoporous materials exhibit outstanding performance in both efficient selective adsorption and recyclability, presenting a novel green adsorbent with promising prospects for sustainable development. This innovation is poised to excel in fields such as sewage treatment, separation, and purification.