X-ray photoelectron spectroscopic (XPS) and secondary ion-mass spectroscopic (SIMS) analyses were performed on unground un-pumiced, unground pumiced, and ground labial enamel surfaces of young bovine incisors exposed to four different treatments: (1) immersion in 35% H2O2 for 60 min; (2) immersion in 37% H3PO4 for 60 s; (3) immersion in 35% H2O2 for 60 min, in distilled water for two min, and in 37% H3PO4 for 60 s; (4) immersion in 37% H3PO4 for 60 s, in distilled water for two min, and in 35% H2O2 for 60 min. Untreated unground un-pumiced, unground pumiced, and ground enamel surfaces, as well as synthetic hydroxyapatite surfaces, served as controls for intra-tooth evaluations of the effects of different treatments. The analyses indicated that exposure to 35% H2O2 alone, besides increasing the nitrogen content, produced no other significant change in the elemental composition of any of the enamel surfaces investigated. Exposure to 37% H3PO4, however, produced a marked decrease in calcium (Ca) and phosphorus (P) concentrations and an increase in carbon (C) and nitrogen (N) concentrations in unground un-pumiced specimens only, and a decrease in C concentration in ground specimens. These results suggest that the reported decrease in the adhesive bond strength of resin to 35% H2O2-treated enamel is not caused by a change in the elemental composition of treated enamel surfaces. They also suggest that an organic-rich layer, unaffected by acid-etching, may be present on the unground un-pumiced surface of young bovine incisors. This layer can be removed by thorough pumicing or by grinding. An awareness of its presence is important when young bovine teeth are used in a model system for evaluation of resin adhesiveness.