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Arsenopyrite (FeAsS) and realgar (As4S4) are two common arsenic minerals that often cause serious environmental issues. Centralised treatment of arsenic-containing tailings can reduce land occupation and save management costs. The current work examined the remediation schemes of tailings from Hunan Province, China, where by different tailings containing arsenopyrite and realgar were blended with exogenous slag zero valence iron (ZVI). Introducing Fe-oxidising bacteria (Acidithiobacillus ferrooxidans) recreates a biologically oxidative environment. All bioleaching experiments were done over three stages, each for 7 days and the solid phase of all tests was characterised by scanning electron microscopy, X-ray diffraction, Fourier-transform infrared spectroscopy, X-ray photoelectron spectroscopy and selective extraction analyses. The results showed that the mixture group reduced arsenic release by 72.9–74.7% compared with the control group. The addition of 0.2 g ZVI clearly decreased arsenic release, and the addition of 4.0 g ZVI led to the lowest arsenic release among all tests. The decrease of arsenic released from the tailings was due to the adsorption and uptake of arsenic by secondary iron-containing minerals and Fe–As(V) secondary mineralisation. The addition of large amounts of ZVI reduced the arsenic detected in the amorphous Fe precipitates. Therefore, a low cost and integrated strategy to reduce arsenic release from tailings is to mix two typical tailings and apply exogenous slag ZVI, which can apply to the in situ remediation of two kinds or more arsenic-containing tailings. [ABSTRACT FROM AUTHOR]