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Direct printing of complex 3D structures at the nano- and microscale is a promising technique for MEMS devices, small-scale sensors, and actuators. So far, most studies have been focused on printing copper (Cu) structures due to the high Coulombic efficiency compared to other conductive metals such as platinum. However, Cu suffers from low material strength, low modulus, and high strain-rate sensitivity. This work introduces a unique Cu-Ni core–shell structure for improved strength. A 3D additive-micromanufacturing technique based on localized electrodeposition was utilized to fabricate dog-bone-shaped Cu micropillars with submicron resolution. These pillars were subsequently coated with Ni by pulse-reverse electrodeposition. A combination of in-situ micropillar compression at various strain rates (0.001–500 s⁻¹) and finite element simulations revealed remarkable strengthening in the Ni-coated Cu …