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[en] A well-dispersed Fe0/Fe3O4/g-C3N4 ternary hybrid composition was successfully synthesized through a calcination route followed by a hydrothermal treatment. It was significant to find that Fe0/Fe3O4/g-C3N4 possesses the optimal photocatalytic efficiency and excellent reusability toward Cr(VI) and RhB. The enhanced photocatalytic efficiency was attributable to the comprehensive factors including intimate contact of Fe0/Fe3O4 with g-C3N4, efficacious recombination inhibition of photoexcited carries, and synergistic interaction between each composition. Moreover, the photoredox catalytic mechanism of Fe0/Fe3O4/g-C3N4 was clearly proved by transient photocurrent responses, PL spectra properties, and exploring the formed active radicals that contribute to the improved photoredox activity. It is expected that our work could offer a notional guidance to design a promising photocatalytic compound for simultaneously degrading heavy metal ions and organic pollutant.