Anionic-cationic switchable monodisperse mesoporous silica nanoparticles were synthesized by one-pot amino and carboxylic acid bifunctionalization based on the self-assembly of the surfactant, two types of co-structure-directing agents containing amino and carboxylic groups, and silica sources. These nanoparticles revealed properties of dispersity and reversibility, with the advantage of the pH-responsive anionic-cationic/acid-base switchability. It was demonstrated that the extracted materials achieved reutilization and controllable dispersity in aqueous solution by adjusting the static electric power among the particles during the switching process.