Positively charged luminescent silica nanoparticles loaded with Tb(III) complex were prepaired by reverse microemulsion procedure with further modification by gemini surfactant. The ξ-potential values and dynamic light scattering data indicate high positive charge and colloidal stability of the as prepaired nanoparticles. The high affinity of these nanoparticles to anions is verified by spectrophotometric measurements with dye molecules, namely phenol red. The insertion of phenol red anions into surfactant bilayer at silica/water interface results in the quenching effect on Tb(III)-centered luminescence of the nanoparticles. Thus "on-off" switching of Tb-centered luminescence indicates the formation of the positively charged bilayer at the silica/water interface. The binding of dodecylsulfate anions with cationic adlayer at the silica/water interface results in the recharging of silica nanoparticles. This recharging can be manifested through the "off-on" luminescent switching, resulted from the displacement of dye anions and reestablishment of Tb(III)-centered luminescence.© (2010) COPYRIGHT SPIE--The International Society for Optical Engineering. Downloading of the abstract is permitted for personal use only.