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A novel Cr-doped BaTiO₃ aerogel was successfully synthesized using a co-gelation technique that involves two metallic alkoxides and a supercritical drying method. This freshly prepared aerogel has a high specific surface area of over 100 m²/g and exhibits improved responsiveness to the simulated sunlight spectrum. Methyl orange (MO) was chosen as the simulated pollutant, and the results reveal that the Cr-doped BaTiO₃ aerogel, when modified with the noble metal silver (Ag), achieves a pollutant removal rate approximately 3.2 times higher than that of the commercially available P25, reaching up to 92% within 60 min. The excellent photocatalytic performance of the Ag-modified Cr-doped BaTiO₃ aerogel can be primarily attributed to its extensive specific surface area and three-dimensional porous architecture. Furthermore, the incorporation of Ag nanoparticles effectively suppresses the recombination of photo-generated electrons and holes. Stability and reusability tests have confirmed the reliability of the Ag-modified Cr-doped BaTiO₃ aerogel. Therefore, this material emerges as a highly promising candidate for the treatment of textile wastewater.