Several biocomposites were synthesized by copolymerizing hydroxyethyl methacrylate (HEMA) and itaconic acid (IA) at varied molar ratios in the presence of different wt% of collagen (CLG) and attapulgite (APG) clay. The structure and properties of the biocomposite adsorbents were characterized by Fourier transform infrared apectroscopy, nuclear magnetic resonance, X‐ray photo electron spectroscopy, X‐ray diffraction, scanning electron microscope, transfer electron microscopy, energy‐dispersive X‐ray analysis, differential thermal analysis–thermogravimetric analysis, point zero charge analysis, mechanical properties, and pH reversibility tests. The synthesis variables were optimized with a central composite design of response surface methodology (RSM). The biocomposite prepared with an optimized composition of 1.5 wt% CLG, 1.7 wt% APG, and 5:1 molar ratio of HEMA:IA showed an adsorption capacity (Qe, mg/g) of 674.4/602.4 for methylene blue (MB)/Rose Bengal (RB) dye from a feed containing 200 mg/L of MB + RB dye mixture in batch mode. In a fixed bed in column mode, the optimized biocomposite showed a removal% of 82.8/71.3 for 100 mg/L inlet concentration, 20 ml/min flow rate, and 20 mm bed height with a breakthrough time of 23/31 min and a mass transfer coefficient (kmtc × 105 cm/s) of 8.36/7.67 for MB/RB as single dye solution.