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The objective of this study was to investigate the chlorine-related challenges in Automotive Shredder Residue (ASR) by developing a de-chlorination strategy and formulating Solid Recovered Fuel (SRF) pellets with improved environmental and fuel quality. A ternary blending approach was employed using Fe–Ca-based inorganic dechlorinating agents and thorny bamboo biomass as co-materials with ASR. The de-chlorination efficiency, calorific value, and ash content of the resulting SRF were evaluated. Results indicated that the optimal dechlorinating formulation reduced the chlorine content of PVC from 43.26 wt% to 0.59 wt%, achieving a de-chlorination efficiency of 97.23%. A second-order polynomial regression model（η_DeCl = –1.5277x² + 2.5519x – 0.0225，R² = 0.9347）was developed to predict the de-chlorination performance based on the blending ratio of dechlorinating agent to ASR, demonstrating behavior consistent with first-order reaction kinetics observed in pyrolytic de-chlorination. The final ternary formulation—comprising 55% thorny bamboo, 37.5% ASR, and 7.5% dechlorinating agent—produced SRF pellets with improved overall quality, demonstrating effective chlorine control, reasonable ash content, and enhanced thermal properties suitable for regulatory compliance and practical application. Such findings meet the criteria set by EN ISO 21640:2021 (Class 2), JIS Z7311 (Grade A), and forthcoming Taiwanese SRF regulations. Based on the findings in this work it can be stated that the high de-chlorination potential of Fe–Ca-based additives for chlorine-rich waste and introduces a predictive formulation model that supports both resource circularity and clean fuel production.