The antimicrobial activity of silver has attracted significant research interest and contributes to an exponentially growing use of this noble metal in commodity products. In this investigation, we describe a general approach to increase the antimicrobial activity of a silver-containing surface by two to three orders of magnitude. The use of 1-2-nm silver particles decorating the surface of 20-50-nm carrier particles consisting of a phosphate-based, biodegradable ceramic allows the triggered release of silver in the presence of a growing microorganism. This effect is based on the organism's requirements for mineral uptake during growth creating a flux of calcium, phosphate, and other ions to the organism. The growing micro-organism dissolves the carrier containing these nutrients and thereby releases the silver nanoparticles. Further, we demonstrate the rapid self-sterilization of polymer surfaces containing silver on calcium phosphate nanoparticles using a series of human pathogens. Colony-forming units (viable bacteria or fungi counts) have been routinely reduced below detection limit and suggest application of these self-sterilizing surfaces in hospital environments, food and pharmaceutical processing, and personal care.