Highly oriented films of the semiconducting transition metal silicide, CrSi 2 , were grown on ( 111) silicon substrates, with the matching crystallographic faces being CrSi 2 ( 001) /Si ( 111). Reflection high-energy electron diffraction (RHEED) yielded symmetric patterns of sharp streaks. The expected streak spacings for different incident RHEED beam directions were calculated from the reciprocal net of the CrSi 2 (001) face and shown to match the observed spacings. The predominant azimuthal orientation of the films was thus determined to be CrSi 2 (2l0>/1Si( 110). This highly desirable heteroepitaxial relationship may be described with a common unit mesh of 51 A 2 and a mismatch of -0.3%. RHEED also revealed the presence of limited film regions of a competing azimuthal orientation, CrSi 2 ( 110) I lSi ( 110). A new common unit mesh for this competing orientation is suggested; it possesses an area of 612 A 2 and a mismatch of -1.2%.