In orthodontic treatment, to achieve efficient tooth movement, it is important to reduce the frictional force between the wire and the bracket, especially the binding friction that occurs when the angle between the wire and the bracket is large. Electroless nickel–polytetrafluoroethylene (Ni-PTFE) coating is a coating technology used to deposit PTFE particles with a low coefficient of friction on the coating surface to provide a low-friction surface for metallic materials. The purpose of this study was to investigate the effect of Ni-PTFE-coated orthodontic wires on the frictional force between brackets. The surface morphology, surface roughness, and frictional properties of Ni-PTFE-coated stainless steel wires and Ni-Ti wires were evaluated. The results demonstrate that the Ni-PTFE coating reduced the frictional force between the orthodontic wires and brackets, despite the increased surface roughness. Even when the angle between the wire and bracket was increased, assuming binding friction, the frictional force was reduced by the Ni-PTFE coating. This suggests that the friction between the wire and the bracket was suppressed by the PTFE particles deposited on the wire surface in contact with the bracket.