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In this work, a Fe-rich nonequiatomic Fe₄₀Cr₁₅Co₁₅Mn₁₀Ni₂₀ high-entropy alloy was successfully prepared based on phase analysis and cost reduction. Fe₄₀Cr₁₅Co₁₅Mn₁₀Ni₂₀ high-entropy alloy with a single-phase face-centered cubic (FCC) structure was strengthened by the addition of 11 at.% Al or 10 at.% Mo, and the variations of phase and mechanical properties of the strengthened alloys were subsequently investigated. It has been found that the addition of 11 at.% Al led to the formation of FCC and body-centered cubic (BCC) dual-phase structure in the Fe₄₀Cr₁₅Co₁₀Mn₄Ni₂₀Al₁₁ alloy, while its yield strength (σ_0.2) and tensile strength increased from 158 ± 4 MPa and 420 ± 20 MPa to 218 ± 7 MPa and 507 ± 16 MPa, respectively, as compared to the single-phase FCC structure Fe₄₀Cr₁₅Co₁₅Mn₁₀Ni₂₀ alloy. The addition of 10 at.% Mo introduced intermetallic compounds of μ and σ phases, which resulted in improved yield strength of 246 ± 15 MPa for the Fe₄₀Cr₁₅Co₁₀Mn₅Ni₂₀Mo₁₀ alloy. However, the alloy exhibited premature brittle fracture due to the existence of a large number of intermetallic compounds, which led to deteriorated tensile strength of 346 ± 15 MPa. The findings of this work suggest that the introduced secondary phases by the addition of Al and Mo can effectively strengthen the high-entropy alloy; however, the number of intermetallic compounds should be controlled to achieve a combination of high strength and good ductility, which provides a reference for the follow-up study of nonequiatomic high-entropy alloys.