The as-cast [Co40Cr25(FeNi)35−yMoy]100−xCx (x = 0, 0.5, y = 3, 4, 5 at.%) HEAs (high-entropy alloys) were prepared by a vacuum arc melting furnace and were then hot rolled. The effect of C and Mo elements on the microstructure evolution and mechanical properties of HEAs was systematically analyzed. The results showed that when no C atoms were added, the HEAs consisted of FCC + HCP dual-phase structure. In addition, as the Mo content increased, the grain size of the alloy increased from 17 μm to 47 μm. However, only the FCC phase appeared after adding 0.5 at.% carbon in Mo microalloyed HEAs, and the grain size of the Mo4C0.5 HEA decreased significantly. Due to the Mo atom content exceeding the solid solution limit, the carbides of Mo combined with the C element appeared in the Mo5C0.5 HEA. The strength of C and Mo microalloyed HEAs significantly increased compared to HEAs with no C added. However, the Mo4C0.5 HEA exhibited excellent comprehensive mechanical properties, which was superior to a majority of reported HEAs and conventional metal alloys. Its yield strength, tensile strength, and elongation were 757 MPa, 1186 MPa, and 69%, respectively. The strengthening mechanism was a combination of fine grain strengthening, TWIP effect, and solid solution strengthening.