The equilibrium‐insoluble Cu and Fe metals with a composition of Cu70Fe30 (at%) are mechanically milled for 20 h, resulting in a metastable single‐phase face‐centered cubic supersaturated solid solution (γS). The alloy powders are consolidated by spark plasma sintering (SPS) at 0.6Tm (622 °C) and 0.7Tm (772 °C), where Tm is the melting point of Cu70Fe30 (1219 °C). Scanning electron microscopy (SEM), X‐ray diffraction (XRD), differential scanning calorimetry (DSC), and electron backscatter (EBSD) analyses are performed on mechanically alloyed powders and SPS bulk samples. Compressive stress–strain and hardness tests are also conducted on the bulk SPS samples to evaluate the mechanical properties. The metallographic study reveals that the γS phase decomposes into Cu‐rich γ and Fe‐rich α phases after SPS. The 0.6Tm sample exhibits a continuous γ‐network phase surrounding an ultrafine γ + α mixture, causing brittle behavior due to crack propagation during compressive testing. In contrast, the 0.7Tm sample features a discontinuous γ‐network phase, enhancing ductility and resulting in a bimodal grain structure. This sample demonstrates superior mechanical properties, combining excellent strength (1056 MPa) and ductility (23%) due to the coexistence of coarser γ‐network grains (1–2 μm) and ultrafine γ + α grains (200–500 nm).
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