Purpose Sediment contamination is complex, and it is challenging to find the solution that corresponds to treating different groups of pollutants effectively. The existence of potentially toxic elements and polycyclic aromatic hydrocarbons in cocontaminated river sediment contributes serious toxic residues to the environment. Thus, it is crucial to involve remediation techniques that simultaneously remove these two complex groups of pollutants. Also, a significant challenge is due to the complex interactions between these groups of contaminants and the sediment matrix. Methods Iron-based materials, such as green produced nano-zero-valent iron, are advantageous, environmentally friendly, and interest in their use is growing. This study demonstrates the potential of green nZVI supported by native clay and biochar for the simultaneous removal of potentially toxic elements and PAHs from co-contaminated river sediment. Results It was indicated that potentially toxic elements removal was better than the removal of PAHs, but the removal of both groups of contaminants was noticeable with no further impact to the environment. The results showed which mechanisms played key roles in removal of pollutants from the river sediment. Additionally, extraction tests showed that sediment treated with modified iron nanoparticles is non-hazardous and that it represented promising results in removal of organic and inorganic pollutants. Conclusion Green synthesis of nZVI by oak leaf extract (Quercus petraea) and supported materials (native clay and biochar) was valuable for recycling wastes and creating treated sediment for potential further beneficial sustainable use.