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To remediate water bodies contaminated with organic micropollutants, recyclable and visible-light-driven coupled photocatalysis-peroxymonosulfate (PMS) activation systems were established by synthesizing magnetic-carbon-nanotubes (CNFe) modified TiO2-x/g-C3N4/CNFe (TCNCNFe) S-scheme heterojunction with oxygen vacancies (O-v) by a simple hydrothermal-calcination approach. The introduction of O-v and CNFe enhances the visible-light-harvesting efficiency and the internal electric field across the heterojunction accompanying favorable energy band bending could effectively migrate the photoexcited electrons along the S-scheme mechanism, thus highly suppressing in situ recombination and improving charge separation. Therefore the TCNCNFe-(30-500)/PMS/Vis system achieved 95.4% removal efficiency of atrazine after 30 min irradiation, meanwhile exhibited excellent recyclability without metal ion leaching due to the unique pod-like nanostructure of CNFe. Moreover, the impacts of certain various reaction variables on pollutant removal were explored to evaluate the practical application potential. Interestingly, the biotoxicity of the treated reaction filtrate was significantly alleviated compared to that of ATZ solution. Furthermore, the exploration of photocatalytic reaction mechanism revealed that the dominant reactive oxidizing species contributed in the following order: h(+) > (OH)-O-center dot > O-center dot(2)- > (SO4-)-S-center dot, and the feasible photodegradation pathway of atrazine was presented based on the determined in-termediates. Hence, this research work holds great promise in ecological environment protection using sustainable solar energy.