Adsorption is a reliable method for removing organic pollutants from water. This article provides data on the use of hybrid composites as adsorbents for Methylene Blue (MB) and Rhodamine 6G (R6G) uptake from aqueous solutions. The organo‐inorganic spherical particles were prepared using tetraethyl orthosilicate and a styrene‐acrylic copolymer through a one‐pot sol‐gel technique. The powder structures were characterised using various methods, including elemental analysis, acid‐base titration, zeta potential measurement, IR spectroscopy, thermogravimetric analysis, low‐temperature nitrogen adsorption, and scanning electron microscopy. The results revealed that the adsorption process demonstrated a preference for a pH of 6 in the case of MB, whereas for R6G, the optimal pH for adsorption was observed to be 7. The findings indicated that the pseudo‐second‐order model accurately described the kinetic data, while the equilibrium data aligned with the Freundlich model. The maximum adsorption capacities were determined to be 212.5 mg/g for MB and 323.1 mg/g for R6G, suggesting that both chemisorption and physical adsorption occurred on the surface of the adsorbent material. The composites were found to be regenerable with an HCl:EtOH mixture up to 3 cycles. These findings suggest that silica/styrene‐acrylic copolymer composites are promising sorbents for removing MB and R6G dyes from aqueous solutions.