Electrodeposited Ni–Fe alloys are expected to have an improved mechanical strength because of their nanocrystalline structure. However, unsatisfactory grain refinement yields a higher coercivity compared with conventional permalloys, which is undesirable in soft magnetic materials. We report electrodeposited Ni–Fe–P alloys that combine the mechanical properties of nanocrystalline materials with soft magnetism that is achievable in coarse-grained permalloys. In Ni–Fe–P alloy electrodeposition, the connections between the bath composition and Fe and P contents of the samples were demonstrated. For Ni–Fe alloys, the introduction of a few percent of P led to a preferable microstructure that was composed of ~10-nm-diameter grains. Up to 2.0 at% P, the resultant Ni–Fe–P alloys achieved a tensile strength of 2.1 GPa, along with a plastic deformability. The electrodeposited alloys exhibited a saturation magnetic flux density of 1.1 T and a coercivity of 8.4 A/m. Our approach indicates that grain refinement by the P alloying can result in a lower coercivity, according to the law of grain size and coercivity.
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