To explore the effects of plasma jet (PJ) and plasma activated water (PAW) on the sterilization of Streptococcus mutans (S. mutans) and compare the advantages and disadvantages of the two methods, so as to provide a basis for plasma treatment of dental caries and to enrich the treatment means of dental caries, an atmospheric pressure plasma excitation system was built, and the effects of PJ and PAW on the sterilization rate of S. mutans and the changes of temperature and pH during treatment were studied under different excitation voltage (Ue) and different excitation time (te). The results showed that in the PJ treatment, the difference in the survival rate of S. mutans between the treatment group and the control group was statistically significant (P = 0.007, d=2.66) when Ue = 7 kV and te = 60 s, and complete sterilization was achieved at Ue = 8 kV and te = 120 s in the PJ treatment. In contrast, in the PAW treatment, the difference in the survival rate of S. mutans between the treatment group and the control group was statistically significant (P = 0.029, d = 1.71) when Ue = 7 kV and te = 30 s, and complete sterilization was achieved with PAW treatment when Ue = 9 kV and te = 60 s. Results of the monitoring of temperature and pH showed that the maximum temperature rise during PJ and PAW treatment did not exceed 4.3 °C, while the pH value after PAW treatment would drop to a minimum of 3.02. In summary, the optimal sterilization parameters for PJ were Ue=8 kV and 90 s < te ≤ 120 s, while the optimal sterilization parameters for PAW were Ue = 9 kV and 30 s<te ≤ 60 s. Both treatment methods achieved non-thermal sterilization of S. mutans, where PJ required only a smaller Ue to achieve complete sterilization, while at pH < 4.7, PAW only required a shorter te to achieve complete sterilization, but its acidic environment could cause some chemical damage to the teeth. This study can provide some reference value for plasma treatment of dental caries.