Epitaxial CrSi2has been successfully grown on (111)Si. Substrate heating at 300 or 400 °C during Cr deposition was found to be more effective than two‐step annealing in promoting the growth and improving the quality of epitaxial CrSi2. The best epitaxy was obtained when sample substrates were heated at 300 or 400 °C followed by 1000–1100 °C annealing for 1 h. The orientation relationships were found to be (0001) CrSi2//(111)Si, (224¯0)CrSi2//(224¯)Si, (202¯0)CrSi2//(202¯)Si, and [12¯13]CrSi2//[101]Si. Dislocations present in the regular interfacial dislocation network were found to be of edge or 60° type with (1)/(6) <112> Burgers vectors. The average dislocation spacings were measured to be 270–320 A˚. The discrepancy of the measured and theoretically expected value of dislocation spacing was attributed to the difference in the thermal expansion coefficients of CrSi2and Si.