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The equiatomic CoCrMnNiFe high-entropy alloy (HEA) has attracted much attention owing to its exceptional mechanical properties. Here, we designed novel face-centered cubic (fcc) phase Co-rich non-equiatomic CoCrMnNiFe HEAs with tensile properties superior to the counterparts, derived from lowering stacking fault energy (SFE) via modifying constituent concentrations. The decrease of Mn, Ni, Fe meanwhile increase of Co, Cr concentrations does reduce the SFE value, based on ab initio and thermodynamics calculations. Hereinto, Co₃₅Cr₂₀Mn₁₅Ni₁₅Fe₁₅ and Co₃₅Cr₂₅Mn₁₅Ni₁₅Fe₁₀ HEAs overcame the strength-ductility trade-off, contributing to twinning-induced plasticity (TWIP) or transformation-induced plasticity (TRIP) effects, respectively. The present study sheds light on developing high performance HEAs.