Single-phase face-centered cubic (fcc) high-entropy alloys (HEAs) exhibits outstanding ductility but low strength, which hinders their practical applications. To overcome this dilemma, we propose a strategy to achieve an excellent combination of high compressive strength and failure strain via controlled formation of hard intermetallic compound in HEAs. Specifically, we vary the Fe content in FeCoMoNi HEAs to control the relative content of μ phase embedded within the ductile fcc matrix and achieve a yield strength of 1877 MPa and an appreciable fracture strain of ~40% in FeCoMoNi HEA. The present work provides deep insight into the design of high-performance HEAs.