This study was based on an industrial sludge landfill with a scale of 1 million cubic meters, which had been filled for more than 10 years. It focused on the secondary dewatering of industrial textile landfill sludge (LS) with a total organic carbon (TOC) content greater than 50% and a volatile suspended solids to suspended solids (VSS/SS) ratio of 0.59. A response surface methodology (RSM) model was established using the coagulant ferrous sulfate (FeSO4) and conditioning agents such as hydrated magnesium oxide (MgO), blast furnace slag (BFS), and calcium oxide (CaO). By solving the RSM equations for the respective indicators, the optimal dosages of FeSO4, MgO, and BFS were determined to be 90 mg/g of dry sludge (DS), and for CaO 174.85 mg/g DS. Further examinations of the dewatering performance, apparent properties, extracellular polymeric substances (EPS) components, rheological characteristics, moisture distribution, and pollutant content variation led to the development of a green waste-based dewatering agent composed of FeSO4 and BFS. In small-scale diaphragm plate and frame filter press tests, the optimal water content (WC) was 69.11%. In the final production-scale experiments, it was 65.72%, with the actual application cost being only 13.07 $/ton DS. Additionally, when FeSO4 and BFS were used together, the combined action of Fe and Si could significantly reduce the biotoxicity of heavy metals (HMs), cut down 75.2% of the LS's TOC, and effectively reduced the leaching of organic substances from the leachate, which was beneficial for subsequent disposal. In conclusion, the combined use of FeSO4 and BFS for the secondary dewatering of industrial textile LS was economically efficient, effective in dewatering, and had significant harm reduction effects, making it a worthwhile for waste treatment.