Thermal spray coatings (TSCs) are widely utilized for limiting degradation of structural components. However, the performance of TSCs is significantly impaired by its inherent non-homogeneous microstructure, comprising of splat boundaries, porosities, secondary phase-formation, and elemental segregation. Herein, we report a simplistic approach for significantly enhancing the corrosion resistance of TSCs. Ni-Cr-5Al2O3 coatings were deposited on stainless steel using high-velocity oxy-fuel technique. The microstructure of as-sprayed coating showed significant inhomogeneities in the form of isolated splats and elemental segregation. The microstructure of developed coatings was modified using a novel processing technique, known as stationary friction processing (SFP). The SFP treatment resulted in complete refinement of coating microstructure with elimination of splat boundaries and pores along with elemental homogenization. The corrosion behavior of as-sprayed and SFP treated coating was evaluated in 3.5\% NaCl solution using potentiodynamic polarization and electrochemical impedance spectroscopy. The SFP treatment reduced the corrosion rate of as-sprayed coating by an order of magnitude. Long-time immersion studies showed continuously decreasing impedance of the as-sprayed coating due to the penetration of the electrolyte along the splat boundaries. In contrast, impedance for the SFP treated coating increased with the immersion time due to the removal of all microstructural defects. Copyright © 2020 American Chemical Society.