Surface preparation is essential to ensure sample homogeneity in terms of surface roughness and mechanical properties, as these factors can significantly affect wear behavior and test repeatability. Although conventional semi-automatic and automatic grinding and polishing processes are efficient and well established, limitations arise for the preparation of large numbers of samples of a hard material such as high-carbon steel, including issues with sample geometry, the need for on-demand sample holders, cost-related limitations, and even considerable human workload and expertise. This study aims to evaluate the use of rotary barrel tumbling—a polishing method that relies on the sliding of abrasive media over the samples’ surface inside a rotating barrel—as an alternative method to prepare the surface of wheel and rail steel samples for pin-on-disc wear testing. A 4-stage tumbling procedure was employed, using different compositions of tumbling media in each stage. Surface roughness and hardness were evaluated throughout the process via 2D and 3D profilometry, microhardness Vickers measurements, and optical microscopy. The proposed method resulted in significant reductions in the surface roughness and hardness of the samples, along with improved homogeneity between samples of different materials and within the same material. These findings suggest that rotary barrel tumbling is an effective alternative method for the surface preparation of pins and discs made of high-carbon steel, enhancing the samples’ suitability for subsequent wear tests.