New experimental data about surface processes of interaction between natural apatite and phosphoric acid solutions were obtained by scanning electron microscopy, Auger electron spectroscopy, and IR reflection spectroscopy. The interaction was found to occur nonstoichiometrically (incongruently) on the very thin surface layer of apatite. The experimental data obtained were compared and extended with results taken from literature. The following sequence of ionic detachment from the surface of apatite to a solution was suggested: first fluorine for fluorapatite or hydroxyl for hydroxyapatite, next calcium, and afterward phosphate. A new chemical mechanism of apatite dissolution was proposed as a result. The mechanism for the first time described the surface irregularity of the dissolution process at the nanolevel. A comparison between this new dissolution mechanism and earlier mechanisms described in the literature was made.