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Hilbert curve patterns were laser-textured on both stainless steel substrates and polytetrafluoroethylene (PTFE) thin coatings by applying 15% and 5% of the 2.3-W full laser power, respectively. The nanomechanical and tribological behavior of both smooth and laser-textured PTFE coatings on both smooth and laser-textured stainless steel substrates were studied. It was found that laser-texturing thin PTFE coatings reduced the hardness of PTFE coatings and prevented the coating from tearing under nanoindenter scratches. Furthermore, laser-texturing on both PTFE coatings and the stainless steel substrate improved the coating wear life 29 times compared to the wear life of the control sample without any laser textures.