Bifunctional SBA-1 mesoporous silica nanoparticles (MSNs) with carboxylic acid and amino groups (denoted as CNS-10-10) have been successfully synthesized, characterized, and employed as adsorbents for dye removal. Adsorbent CNS-10-10 shows high affinity towards cationic and anionic dyes in a wide pH range, and exhibits selective dye removal of a two-dye mixture system of cationic methylene blue and anionic eosin Y. By changing the pH of the medium, the selectivity of the adsorption behavior can be easily modulated. For comparison purposes, the counterparts, that is, pure silica SBA-1 MSNs (CS-0) and those with either carboxylic acid or amino functional groups (denoted as CS-10 and NS-10, respectively) were also prepared to evaluate their dye-adsorption behaviors. As revealed by the zeta-potential measurements, the electrostatic interaction between the adsorbent surface and the dye molecule plays an important role in the adsorption mechanism. Adsorbent CNS-10-10 can be easily regenerated and reused, and maintains its adsorption efficiency up to 80 % after four cycles.