The modern dentifrice industry needs non-toxic materials able to adhere to dentin, occlude dentinal tubules, hold pharmacons at the surface of dentin, and release them on demand to the location the tooth needs them most. Novel dental materials loaded with eugenol or fluoride-ions examined for the release of the pharmacon in an aqueous suspension efficiently adhere to the surface of human dentin and occlude dentinal tubules as evidenced by Scanning Electron Microscopy (SEM). Ultraviolet-visible (UV-vis) absorption spectroscopy and a fluoride-selective electrode quantified the release of pharmacons. The surface modification with casein stabilizes micro- and nanoparticles of calcium carbonate in aqueous suspensions, enabling their application in dentifrices. The ability of particles to hold and release eugenol depends on their morphology and composition, with the casein-coated calcium carbonate microspheres being the most acid-sensitive and most promising for dentifrice applications. The novel material releases fluoride under physiologically low pH, regardless of the presence of other ingredients of the artificial saliva, which sustains the bulk fluoride concentration comparable with most fluorinated toothpastes. Low pH-triggered release mechanisms selectively supply the drug to the areas that need it most, reducing the overall dose and ushering in a new type of targeted dentifrices.