This study investigated the effects of a diamond-like carbon (DLC) coating on frictional and mechanical properties of orthodontic brackets. DLC films were deposited on stainless steel brackets using the plasma-based ion implantation/deposition (PBIID) method under two different atmospheric conditions. As-received metal brackets served as the control. Two sizes of stainless steel archwires, 0.018 inch diameter and 0.017 × 0.025 inch cross-section dimensions, were used for measuring static and kinetic friction by drawing the archwires through the bracket slots, using a mechanical testing machine (n = 10). The DLC-coated brackets were observed with a scanning electron microscope (SEM). Values of hardness and elastic modulus were obtained by nanoindentation testing (n = 10). Friction forces were compared by one-way analysis of variance and the Scheffé test. The hardness and elastic modulus of the brackets were compared using Kruskal–Wallis and Mann–Whitney U-tests. SEM photomicrographs showed DLC layers on the bracket surfaces with thickness of approximately 5–7 μm. DLC-coated brackets deposited under condition 2 showed significantly less static frictional force for the stainless steel wire with 0.017 × 0.025 inch cross-section dimensions than as-received brackets and DLC-coated brackets deposited under condition 1, although both DLC-coated brackets showed significantly less kinetic frictional force than as-received brackets. The hardness of the DLC layers was much higher than that of the as-received bracket surfaces. In conclusion, the surfaces of metal brackets can be successfully modified by the PBIID method to create a DLC layer, and the DLC-coating process significantly reduces frictional forces.