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Although various processes for metal printing at the micro- and mesoscale have been demonstrated, printing functional devices such as thermocouples, thermopiles, and heat flux sensors that function based on interfaces between an alloy and another alloy/metal demands processes for printing alloys. Furthermore, a high-quality and crystalline alloy is required for acceptable function of these devices. This article reports for the first time co-electrodeposition-based printing of single-phase solid solution nanocrystalline copper/nickel (Cu/Ni) alloy with various controllable compositions (Cu100Ni0 to Cu19Ni81) from a single electrolyte. The printed alloy is nanocrystalline (<35 nm), continuous, and dense with no apparent porosity, with remarkable mechanical and magnetic properties, without any postprocessing annealing such as heat treatment. In addition, a functional thermocouple fabricated using this process is …