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Several laser systems for the removal of hard dental substances are currently under investigation. However, in most cases, such systems have been demonstrated to be inefficient or have led to undesirable thermal side-effects. This paper reports, for the first time, the removal of enamel and dentin by a picosecond laser system, a solid-state Nd:YLF laser. Very precise cavities can be obtained in the enamel and dentin of extracted human molars when laser pulses are distributed onto well-defined areas of the teeth. Scanning electron microscopy shows that the quality of the cavities is superior to that achieved by other laser systems. The cavity walls are very steep, and their surfaces are characterized by a sealed structure. In contrast to laser systems with longer-duration pulses, picosecond laser pulses ablate with less thermal damage to the surrounding substance. The results of dye penetration tests and polarized microscopy show that even mechanical shock-wave effects are negligible. When the Nd:YLF laser is applied to carious enamel, the ablation rate is found to be about ten times higher than for sound molars, thus making the Nd:YLF laser a caries-selective laser system.