A low-temperature hydrothermal process was developed to synthesize erdite adsorbent from a solid waste sludge contained 10.2% Fe, 6.2% Al and 1.4% Si, alongside 59.5% water content. At 90℃, adding Na₂S and NaOH could convert it into erdite nanorods with a diameter of 80 nm and a length of 100 nm. In the sludge, only Fe oxyhydroxide was involved in the formation of erdite, and the other Al/Si-bearing compounds were dissolved in an alkaline medium. The dissolved Al/Si-bearing compounds were further removed, forming faujasite so that the used medium was purified and then entirely recycled into the next conversion stage. No secondary waste was generated in the pilot-scale conversion, and the adsorption efficiency of the prepared products to wastewater with a high initial Cr(VI) concentration of 1000 mg/L was more than 99.5%. The adsorption data complied with the pseudo-second-order kinetics. During the wastewater treatment, hexavalent chromium anion diffused to erdite surface and replaced single bondOH/single bondSH groups of adjacent structural Fe to form a stable complex ligand. In addition, the redox reaction between hexavalent chromium and the -SH group occurred to generate a trivalent chromium complex on the Fe/S-bearing flocs surface.