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In this study, a special core–shell structured wool-TiO₂ (WT) hybrid composite powder also having TiO₂ nanoparticles incorporated inside cortical cells was reported. The wool pallets were pulverized from wool fibers using vibration-assisted ball milling technique and the WT powders having mesopores and macropores were produced in hydrothermal process. Experimental results indicated that the infiltrated TiO₂ nanoparticles were amorphous structure, while the coated TiO₂ nanoparticles were anatase phase structure. The crystallized TiO₂ nanoparticles were grafted with wool pallets by the N−Ti⁴⁺/S−Ti⁴⁺/O−Ti⁴⁺ bonds. The BET surface area was measured as 153.5 m²/g and the particle sizes were in the 600–3600 nm and 4000–6500 nm ranges. The main reactive radical species of the WT powders were holes, and •O₂⁻, ¹O₂, and •OH were also involved in the photodegradation of MB dye under visible light irradiation. The experimental parameters for photodegradation of MB dye solution were optimized as follows: 0.25 g/L of WT powders was added in 40 mL of 3 mg/L MB dye solution containing 50 mL/L H₂O₂, which resulted in the increases of COD value of degraded MB dye solution up to 916.9 mg/L at 120 min. The WT powders could be used for repeatedly photodegradation of both anionic and cationic dyes.