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Laser powder bed fusion (L-PBF) additive manufacturing was utilized to fabricate high-strength copper (Cu) alloys through inoculation of pure Cu powder with cobalt (Co) submicron particles. It was found that when the addition level of Co is lower than its maximum solid solubility in Cu (4.75 wt.%), the microstructure of Cu-Co alloys is characterized by coarse columnar grains. Further addition of Co over 4.75 wt.% led to a heterogeneous grain structure, with large equiaxed grains or columnar grains near the centers of melt pools whereas ultrafine equiaxed grains sitting on the melt pool boundaries. Microstructure characterization showed that the in-situ formed dual phase nanoparticles with Co shell and cobalt oxide (CoO) core acted as heterogeneous nucleation sites of Cu, which allowed ultrafine, equiaxed grains to form. The heterogeneously structured as-built Cu-Co alloy achieved a tensile strength of 381.4 ± 2.9 …