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Emerging pollutants and a large volume of unused dyes from the textile industry have been contaminating water bodies. This work introduces a scalable approach to purifying water by the adsorption of Acid green 25 (AG), Crystal Violet (CV), and Sulfamethoxazole (SMA) from an aqueous solution by graphene oxide (GO) doped modified silica aerogel (GO-SA) with supercritical fluid deposition (SFD) method. Characterization of GO-SA using X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR), high-resolution scanning electron microscopy (HR-SEM), thermogravimetric analysis (TGA), and Brunauer–Emmett–Teller (BET) adsorption isotherms revealed the improvement in the adsorbent surface area, and its textural properties. The high removal percentages observed in most of the experimental runs provide evidence of the excellent performance of the adsorbent towards the anionic and cationic dyes along with the antibiotic. The adsorption isotherm and kinetics showed that the Langmuir isotherm and pseudo-second-order kinetic models could explain adsorption. The adsorbent holds a higher adsorption capacity for SMA (67.07 mg g−1) than for CV (41.46 mg g−1) and AG (20.56 mg g−1) due to the higher hydrophobicity that interacts with the hydrophobic adsorbent. The GO-SA successfully removed AG, CV, and SMA with removal percentages of 98.23%, 98.71%, and 94.46%, respectively. The parameters were optimized using Central Composite Design (RSM-CCD). The prepared aerogel showed excellent reusability with a removal efficiency of > 85% even after 5 cycles. This study shows the potential of GO-SA adsorbent in textile and other wastewater purification. [ABSTRACT FROM AUTHOR]