We have investigated the work softening (WS) phenomena during a cold-roll process of an Al-Fe alloy, based on hardness measurements, electron microscopy observations, and thermodynamic calculations. The WS behavior was con rmed in the Al-Fe alloy when the rolling rate was larger than 80%, which contained ne grains with severe deformation. In contrast, the behavior and microstructural features were hardly observed in the A1050 alloy. Composition analyses showed that almost all Fe in the present Al-Fe alloy form the θ-Al 13 Fe 4 phase, in which a trace impurity element, Si, is found to be signi cantly segregated. This Si partitioning behavior is con rmed by the thermodynamic calculations and consequently leads to a higher puri cation of the relevant Al matrix as being almost close to the 4N (99.99 mol%) level, known as a scavenging effect of the impurities. It can be concluded that the highly puri ed aluminum matrix provides an intrinsic origin of the WS of the present Al-Fe alloy. Signi cant reductions of the impurities may lead to an extended mean-free path of dislocation motions and related grain boundary effects, which promote the occurrence of dynamic recovery and/or recrystallizations at severe deformation ranges even during the cold-roll process.