The sintered copper-based friction materials for high-speed train brake pads have a complex composition that should possess good physical, mechanical, and tribological properties in practical applications. For this article, four kinds of friction materials were prepared by powder metallurgy technology and the effects of iron powders on the microstructural and tribological properties of copper-based friction materials were characterized using a scanning electron microscope (SEM) and x-ray diffraction (XRD). The results showed that iron powder as an enhancing component could effectively change the friction and wear properties of the experimental materials. The copper-based friction materials containing hydroxy iron (1–5 μm) have a relatively higher coefficient of friction: The friction coefficient was significantly improved by 16.8% compared with reduced iron under a rotation speed of 4000 r/min. The friction coefficient of friction material containing water-atomized iron powder is relatively reliable with 3000–7000 r/min speed range. In a high-speed environment, the friction surface of material containing reduced iron or hydroxy iron (1–5 μm) mainly has cracks and brittle fractures, and the material containing hydroxy iron (10 μm) or water-atomized iron has an obvious layered structure and shows fatigue wear.