The nanoscale precipitation and the mechanical properties of the two CuNiAl-containing steels with different Cu contents aged at 500 °C were investigated in this study. Results of mechanical property indicated that the co-precipitation of Cu-rich and NiAl phases during aging contributed to the precipitation strengthening effects. The influence of Cu content on the evolution of precipitates was studied by atom probe tomography (APT). The results demonstrated that the increasing of Cu content enhanced the number density of precipitates and accelerated the precipitation process. The two steels showed two kinds of precipitation sequences on account of different Cu contents. The steel 1 with low Cu content exhibited a precipitation sequence of “supersaturated solid solution → NiAl → NiAl + Cu”, while the steel 2 with high Cu content presented the process of “supersaturated solid solution → Cu → Cu + NiAl”. After further aging, the precipitates of both steels were transformed into Cu/NiAl co-precipitates without isolated Cu-rich phases and isolated NiAl phases. • Hardness of the CuNiAl-containing steel can be improved by increasing the Cu content. • The increasing of Cu content enhances the number density of precipitates and accelerates the precipitation process. • The precipitation sequences of two steels with different Cu contents are clarified.