In this study, an ultrasonic nanocrystalline surface modification (UNSM) technique was applied to normal and heat-treated rails made of 60 kgK steel to enhance the wear resistance of the wheel-rail interaction. The hardness and compressive residual stress values of the untreated and UNSM-treated rails were measured by the Brinell hardness tester and X-ray diffraction technique, respectively. It was found, according to the measurement results, that the hardness was increased by about 20% and 8%, whereas the compressive residual stress was induced by about 52% and 62% for the UNSM-treated normal and heat-treated rails, respectively. The UNSM-treated normal rail showed a slightly higher hardness than the heat-treated rail. The wear resistance of rails with respect to rotating speed and rolling time was assessed using a rolling contact wear (RCW) tester under dry conditions. The RCW test results revealed that the wear of the UNSM-treated rails was enhanced in comparison with those of the untreated rails. Also, the wear amount of the rails was increased with increasing the rotation speed. The UNSM-treated normal rail exhibited the highest wear resistance with respect to the rotation speed. The wear mechanisms of the rails are also discussed based on microscopic images of the worn out surfaces.