Using a combination of an aqueous layer-by-layer deposition technique, nanoparticle surface modification chemistry, and nanoreactor chemistry, we constructed thin film coatings with two distinct layered functional regions: a reservoir for the loading and release of bactericidal chemicals and a nanoparticle surface cap with immobilized bactericides. This results in dual-functional bactericidal coatings bearing both chemical-releasing bacteria-killing capacity and contact bacteria-killing capacity. These dual-functional coatings showed very high initial bacteria-killing efficiency due to the release of Ag ions and retained significant antibacterial activity after the depletion of embedded Ag because of the immobilized quaternary ammonium salts.