The removal of dyes from wastewater that are released during industrial processes has become a significant concern in the environmental science in recent years. To tackle this issue, researchers are exploring the use of nanomaterials for designing new adsorbents. Another promising approach is to grow polymer brushes with high density functional groups via surface-initiated atom transfer radical polymerization (SI-ATRP), which can significantly enhance their ability to absorb dyes. The presence of carboxylic acid groups on the adsorbent material significantly contributes to its efficacy in dye removal by enhancing adsorption capacity, enabling selective adsorption, pH-dependent behavior, chelation, or complexation, and providing stability for repeated usage. In this work, a nanomaterial of carboxylic functionalized poly (methacrylic acid 2-(tert-butylamino)ethyl ester)-coated mesoporous silica nanoparticles (MSNPs–PMATBAE–COOH) was synthesized by the growth of PTBAEMA via surface-initiated atom-transfer radical polymerization, then reacted with succinic anhydride reaction. The chemical structure of MSNPs–PMATBAE–COOH was confirmed using multiple methods, including FT-IR and DLS, and the core-brush morphology was observed clearly using TEM. MSNPs–PMATBAE–COOH were subsequently employed to adsorb hazardous dyes efficiently. The anionic polymer brushes enabled the adsorption of methylene blue (MB) and tetraethylrhodamine (TER) at optimum pH value of 3. The results also indicated that MSNPs–PMATBAE–COOH possessed significant adsorption capacity (263.4 and 212.9 mg g−1 for MB and TER, respectively) and fast adsorption rate (within 15 min), which can be explained by the abundance of adsorptive polymer brushes and the small size of the nanoparticles. Overall, the findings indicate that MSNPs-PMATBAE-COOH is a highly effective adsorbent material for eliminating dye pollutants from wastewater.