The impact of cold atmospheric plasma (CAP) treatment on the enamel of twelve primary teeth (incisors, canines, and molars) collected from six children was examined in order to evaluate the possibility of using the CAP technique in dental applications. A radio-frequency dielectric barrier discharge (DBD) plasma jet operating at a voltage of 3.25 kV using a mixture of helium and oxygen as the working gas was used for the generation of plasma as part of the electro-technological method for the treatment of biological material. The plasma exposure time for the primary teeth was 5, 10, and 20 min. The properties of tooth enamel (color, contact angles, surface roughness, surface topography, elemental composition) were examined before (control) and after the plasma treatment. As shown by the results, the plasma treatment time is a key parameter that can induce desired features, such as whitening or improved wettability. However, with prolonged plasma treatment (20 min), the enamel surface may be permanently damaged. The cold-plasma-treated samples were characterized by a higher value of the brightness L* parameter and thus a lighter color, compared to the CAP-untreated teeth. It was also evidenced that the plasma treatment increased the hydrophilicity of tooth surfaces, and the contact angles effectively decreased with the time of the CAP treatment. The tooth surface also became much more heterogeneous and rough with much greater amplitudes in heights. The surface of the primary teeth after the CAP treatment lost its homogeneity, as evidenced by the SEM micrographs. The analysis of the elemental composition revealed only minor changes after the plasma process, which may suggest that the observed morphological changes in the enamel surface are mainly physical and are not a consequence of chemical reactions between the enamel and the reactive components of the cold plasma. Plasma treatment of teeth opens up new possibilities of using this method as an alternative to whitening or pre-treatment before other dental procedures.