The influence of various Fe contents (5, 10, 20, and 40 wt.%) on the microstructure and properties of powder metallurgy Cu-Fe alloy by spark plasma sintering, subjected to cold rolling and aging treatments, was explored. The results showed that, with increasing Fe content from 5 wt.% to 40 wt.%, the distribution of Fe phase evolved from the discrete spheroid to the continuous stagger, accompanying with its size increasing from 0.29 to 1.20 μm. Accordingly, the yield strength of the aged alloy increased from 411.5 to 788.8 MPa, whilst the electrical conductivity decreased from 62.5% (IACS) to 42.0% (IACS). Moreover, a rule of mixture was proposed to calculate the contribution of Cu matrix, primary Fe phase and secondary Fe phase to the yield strength of the alloy, which works well in the prediction of mechanical properties for Cu-Fe alloys with Fe content higher than10 wt.%.