Abstract: Self-lubricating materials with solid lubricants are essential for the design of friction pairs. However, solid lubricating phases inevitably reduce the mechanical properties of materials, limiting the improvement of their tribological properties. Studies had shown that among lead -free Cu-based self-lubricating composites, FeS/Cu–Bi materials had better antifriction and wear characteristics. Bi and FeS showed a good synergistic lubrication effect in terms of their antifriction and antiadhesion properties. However, FeS is easy to agglomerate and has poor wettability with copper alloys, the introduction of an FeS lubricating phase into the copper matrix destroys the continuity of the metal matrix, and poor interface bonding occurs between FeS and the Cu matrix, which substantially reduces the mechanical properties and reliability of the materials. Consequently, the tribological and mechanical properties of FeS/Cu–Bi composites cannot be fully developed and utilized. To enhance the mechanical and tribological properties of copper-based self-lubricating materials, this work adopted a strategy combining copper-plated steel fibers and shift-speed ball milling alloying and successfully prepared FeS/Cu–Bi self-lubricating materials through powder metallurgy to enhance the mechanical and tribological properties of copper-based self-lubricating materials. The microstructure of the materials was characterized by scanning electron microscopy. Tests on the crushing strength, impact toughness, and tribological properties of the materials were conducted using a universal electronic testing machine, a 300 J pendulum impact testing machine, and an M200 ring-block sliding tribometer, respectively. Results showed that the mechanical properties of the materials first increased and then stabilized with an increase in the copper-plated steel fiber length. When the length of the copper-plated steel fiber was 7 mm, the mechanical properties of the material reached stability. Compared with the material without a copper-plated steel fiber, its crushing strength and impact toughness were increased by 32.6% and 53%, respectively. As the length of the copper-plated steel fibers increased, the friction coefficient and wear rate of the materials decreased and then rised. Short copper-plated steel fibers existed as hard particles in the material, and the mechanical properties of the material were poor. Short copper-plated steel fibers increased the friction resistance between the material and the counterpart, which was not conducive to the retention and spreading of FeS and Bi on the friction surface and exacerbated the adhesion and plowing wear of the material. When the length of copper-plated steel fibers was excessively long, that was, 11 mm, their extensive spreading in the copper matrix increased the direct contact with the counterpart, reduced the materialʼs antifriction characteristic and wear resistance, and led to increased plowing wear on the material surface. The comprehensive mechanical and tribological properties of the copper-plated steel fiber material with a length of 7 mm were optimal, which could achieve a unity of high strength and good self-lubricating properties, and improve the friction reduction and wear resistance of the material by 17.6% and 55%, respectively. This research provided new ideas for improving the comprehensive mechanical and tribological properties of solid self-lubricating materials.