Recent studies have shown that carbon nanotubes (CNTs) can be used as biomedical materials because of their unique properties. CNTs effect nucleation of hydroxyapatite, because of which considerable interest has been generated regarding the use of CNTs in dentistry. However, there are only a few reports on the use of CNTs as dental materials. In this study, we investigated the changes induced in the surfaces of tooth slices by the application of a coating of CNTs by observing CNT-coated tooth slices both macroscopically as well as under a scanning electron microscope. Further, we investigated the effect of CNT coating on the tensile bond strength of dentin adhesives. CNTs adhered easily to the tooth surfaces when tooth slices were suspended in a CNT-dispersed solution. Interestingly, it was observed that CNTs selectively adhered to the surfaces of dentin and cementum, possibly by adhering to their exposed collagen fibers. In addition, the CNT coating did not affect the tensile bond strength of dentin adhesives. These results indicate that coating of the teeth with CNTs can be a possible application of CNTs as dental materials.