In-situ neutron diffraction measurements were performed on a cold-rolled copper-iron (Cu-Fe) alloy during tensile tests at 293 K and 150 K. The alloy was composed of face-centered cubic Cu and body-centered cubic Fe. The roles of Cu and Fe on the deformation behavior of alloys were discussed and clarified. The strength and work-hardening rate of the alloy increased with decreasing test temperature. Furthermore, the phase stress of Fe increased considerably with decreasing test temperature; however, the response of this stress to the applied true stress exhibited no dependence on the temperature. The phase stresses of Cu changed only slightly with decreasing test temperature. However, the Cu phase stress response to the applied true stress increased with decreasing test temperature, indicating an increase in the work-hardening rate. The strengthening of Fe and the increase in the work-hardening of Cu contributed to an increase in the strength and work-hardening rate of the Cu-Fe alloy at low temperatures.