Textile industries release dyes into wastewater, and when present above certain levels, these dyes pose serious risks because of their high toxicity. This study investigates the removal of Sunset Yellow (SY) and Methylene Violet (MV) dyes from wastewater using chitosan (CS) and polysilicate acid (pSi) in the structure of aluminum-based coagulants, resulting in hybrid formulations (CS@Al, Al/pSi, and CS@Al/pSi). Among the various treatment methods that have been applied for the removal of dyes, the coagulation/flocculation process was chosen in the present study, as it is a cheap and effective method. Coagulation performance was optimized for pH, coagulant dosage, temperature and mixing time. The Al/pSi coagulant achieved nearly complete SY removal (98.8%) at 25 mg/L dosage and pH 3.0. MV removal in single-dye solutions was limited, with Al/pSi achieving only 26.6% removal at pH 3.0. However, in mixed-dye systems (SY/MV), synergistic interactions increased MV removal up to 94.4% and SY removal to 100%. Hybrid CS@Al/pSi showed lower SY removal (36.4%) for SY at 50 mg/L but provided stable floc formation, particularly in mixtures of anionic and cationic dyes. Application to real textile wastewater confirmed the high efficiency of the optimized coagulants, particularly with Al/pSi_20,A and AlCl₃, indicating their potential for industrial wastewater treatment. SEM, EDS, XRD, and FTIR analyses revealed structural consolidation, increased surface area, and successful dye adsorption, explaining the high removal efficiency.