The interaction of an Nd:YAG laser, operating at 532 nm with 40 ps pulse duration, with human teeth was studied. The results show that teeth were significantly modified at an energy fluence of about 11 J/cm2. Various surface morphologies of enamel and dentine were recorded. Features on enamel include crater (conical form) in the central part and cauliflower morphology at the periphery, whereas on dentine the crater looks like a stretched dome between sharp edges. The behavior of the enamel-dentine junction area showed different morphology with respect to both tooth enamel and dentine alone. Finally, the junction channel showed a removal of collagen fibers and the formation of a needle-like bottom structure. Generally, this investigation showed that the picosecond Nd:YAG laser can ablate a tooth surface practically instantaneously, implying that large tooth surfaces can be processed in short time.