Total hip arthroplasty (THA) is a surgical procedure for patients with pain and difficulty walking due to hip osteoarthritis. In primary THA, the acetabulum and femoral head are replaced by a prosthesis where the modular femoral head and inner liner of the acetabulum form the bearing surface. The most popular bearing surface used in the United States, metal-on-polyethylene, consists of a cobalt–chromium molybdenum (CoCrMo) alloy femoral head that articulates with a polyethylene acetabular liner, typically made of highly cross-linked polyethylene. While successful in most cases, THA sometimes fails, commonly from aseptic loosening due to the wear debris of polyethylene. Fine-particle shot peening (FPSP) is a simple method for enhancing the mechanical properties and surface properties of metal, including reducing friction and enhancing the lubrication properties of the metal surface. In this study, we applied FPSP to the CoCr in the femoral head of a hip prosthesis to improve its surface properties and conducted experiments with pin-on-disc tribometers using CoCr as a pin and highly cross-linked polyethylene as a disc to mimic the THA implant. The results show that FPSP significantly enhances the tribological properties of the CoCr surface, including lubrication; decreases the friction coefficient; and decreases the polyethylene wear volume.