Dyeing industries release their hazardous dyeing effluents into the environment which affects the human health and ecosystem. Hence, the removal of dye from waste‐water is mandatory one. In this present study, focus on the fabrication of bio‐clay‐ceramic hybrid composites by dispersing bentonite (BT) clay and ceramic hydroxyapatite (HA) into alginate (Alg) and gelatin (Gel) polymeric matrixes by in‐situ method which gives BTHAAlg and BTHAGel hybrid composites for methylene blue (MB) removal. The various adsorption influencing parameters such as shaking time, adsorbent dosage, pH and initial MB concentration were optimized under batch method. The highest MB adsorption capacities of BTHAAlg and BTHAGel composites were found to be 43.70 and 47.50 mg/g respectively with optimized conditions of 100 mg/L of initial MB concentration, 40 min shaking time and 0.1 g dosages. In pH studies, the high MB adsorption capacity of bio‐clay‐ceramic composites were noticed at pH 11. The characterization techniques like FTIR, SEM and EDAX analysis were performed to find the physico‐chemical properties of bio‐clay‐ceramic composites. The equilibrium data of hybrid composites towards MB adsorption was well fitted with Langmuir isotherm model than D‐R and Fruendlich models because of higher r and low sd values. The negative values of ▵Go at three different temperatures (303, 313 and 323 K) indicate that the spontaneous nature of MB adsorption, while positive values of ΔHo and ΔSo revealed that the MB adsorption onto hybrid composites was endothermic in nature and more randomness occurred at solid/liquid interfaces. In kinetic studies, the MB adsorption onto hybrid composites was well fitted with pseudo‐second‐order and intra‐particle diffusion models. The electrostatic attraction and hydrogen bonding plays a dominant role in MB adsorption onto BTHAAlg and BTHAGel bio‐clay‐ceramic composites. The regeneration studies proposed that the hybrid composites can be reusable upto five cycles. Hence, the developed bio‐clay‐ceramic hybrid composites were act as best adsorbents for MB removal.
