In this technical brief, a Cr3Si nanocrystalline film was deposited on 304 stainless steel (SS) substrate using a double glow discharge plasma technique. The film was characterized by X-ray diffraction, scanning electron microscopy (SEM), transmission electron microscopy, nanohardness tester, and scratch tester. The as-deposited film with a thickness of 5 μm consisted of A15 structured Cr3Si phase with an average grain size of 8 nm. The hardness values of the film were determined to be 26 GPa, which was ten times greater than 304 SS. A self-designed ultrasonic vibration cavitation erosion apparatus was employed to evaluate the cavitation erosion resistance of the Cr3Si film. The results showed that after cavitation tests of 30 hrs, the erosion mass loss of the film was only 60% of that for 304 SS substrate. SEM observation of the erosion surfaces indicated that the surface damage degree of the Cr3Si film is significantly less than that of 304 SS.