Electropolishing at high current densities without agitation of the electrolyte results in a pitting phenomenon that produces dimple-like surface features. Although pitting is unfavorable in the electropolishing process, its effect on surface modification, such as surface texturing, has not been thoroughly investigated. Surface topography and chemical composition analyses of electropolished steel revealed surface pits and an oxide surface layer, indicating the presence of surface texture and coating. The resulting surface is characterized by negative skewness and high kurtosis values. The tribological behavior of the electropolished steel-bronze pair is investigated by evaluating coefficients of friction and bronze wear using sliding tests conducted in mixed and boundary lubrication regimes. The results are compared to those of the ground steel-bronze pair. In the mixed and upper range of the boundary lubrication regime, coefficients of friction reduction up to 30% and shorter running-in phases are observed for electropolished steel (electropolished steel μ avg = 0.019 vs. ground steel μ avg = 0.028). In contrast, the coefficient of friction increased in the lower range of boundary lubrication regime by 50% (electropolished steel μ avg = 0.098 vs. ground steel μ avg = 0.065). Electropolishing, as a cost- and time-effective method applicable to complex geometries, presents an alternative method for achieving surface modifications aimed at friction reduction and improved tribological behavior for non-conformal contacts in the boundary and mixed lubrication regimes.