Microstructure and mechanical properties of non-equiatomic (CuNi)100−xCox (x=15, 20, 25 and 30, at.%) medium-entropy alloys (MEAs) prepared by vacuum arc-melting were investigated. Results show that all the as-cast MEAs exhibit dual face-centered cubic (fcc) solid-solution phases with identical lattice constant, showing typical dendrite structure consisting of (Ni, Co)-rich phase in dendrites and Cu-rich phase in inter-dendrites. The positive enthalpy of mixing among Cu and Ni-Co elements is responsible for the segregation of Cu. With the increase of Co content, the volume fraction of (Ni, Co)-rich phase increases while the Cu-rich phase decreases, resulting in an increment of yield strength and a decrement of elongation for the (CuNi)100−xCox MEAs. Nano-indentation test results show a great difference of microhardness between the two fcc phases of the MEAs. The measured microhardness value of the (Ni, Co)-rich phase is almost twofold as compared to that of the Cu-rich phase in all the (CuNi)100−xCox MEAs. During the deformation of the MEAs, the Cu-rich phase bears the main plastic strain, whereas the (Ni, Co)-rich phase provides more pronounced strengthening.