A surface of an article is modified by first disposing a nickel-enriched region at the surface of a substrate, then enriching the nickel-enriched region with aluminum to form an aluminized region, and finally removing at least a portion of the aluminized region to form a processed surface of the substrate. Upon removal of this material, the roughness of the surface is reduced from a comparatively high initial roughness value to a comparatively low processed roughness value. In some embodiments, the processed roughness is less than about 95% of the initial roughness. Moreover, the sequence of steps described herein may be iterated one or more times to achieve further reduction in substrate surface roughness.