Flexspline frictional degradation causes failure of harmonic drives. This study focused on the improvement of the flexspline tribological properties. Flexspline material 40Cr was modified with a robust polydimethylsiloxane (PDMS) coating. Etched and chemically modified films were utilized to enhance the organic PDMS coating-substrate link strength. Comparing modified and unmodified 40Cr, the surface friction coefficient decreased by 82.2%. Moreover, the modified 40Cr exhibited excellent load-bearing properties. The effects of speed and lubricant-coating interaction on the tribological properties were verified. This study provides an essential theoretical basis for improving the tribological performance of harmonic drives via soft coating modification.