Reducing the friction force between the commercial archwire and bracket during the orthodontic treatment in general dental practice has attracted worldwide interest. An investigation on the friction and wear behaviors of the uncoated and carbon film coated stainless steel archwires running against stainless steel brackets was systematically conducted. The carbon films were prepared at substrate bias voltages from +5 to +50 V using an electron cyclotron resonance plasma sputtering system. With increasing substrate bias voltage, local microstructures of the carbon films evolved from amorphous carbon to graphene nanocrystallites. Both static and stable friction coefficients of the archwire-bracket contacts sliding in dry and wet (artificial saliva) conditions decreased with the deposition of carbon films on the archwires. Low friction coefficient of 0.12 was achieved in artificial saliva environment for the graphene sheets embedded carbon (GSEC) film coated archwire. Deterioration of the friction behavior of the GSEC film coated archwire occurred after immersion of the archwire in artificial saliva solution for different periods before friction test. However, moderate friction coefficient of less than 0.30 sustained after 30 days immersion periods. The low friction mechanism is clarified to be the formation of salivary adsorbed layer and graphene sheets containing tribofilm on the contact interfaces. The robust low friction and low wear performances of the GSEC film coated archwires make them good candidates for clinical orthodontic treatment applications.