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A cost-effective, scalable and versatile method of preparing nano-ink without hazardous chemical precursors is a prerequisite for widespread adoption of printed electronics. Precursor-free synthesis by spark discharge is promising for this purpose. The synthesis of platinum nanoparticles (PtNPs) using a spark discharge under Ar, N2, and air has been investigated to prepare highly conductive nano-ink. The size, chemical composition, and mass production rate of PtNPs significantly depended on the carrier gas. Pure metallic PtNPs with sizes of 5.5 ± 1.8 and 7.1 ± 2.4 nm were formed under Ar and N2, respectively. PtNPs with sizes of 18.2 ± 9.0 nm produced using air consisted of amorphous oxide PtO and metallic Pt. The mass production rates of PtNPs were 53 ± 6, 366 ± 59, and 490 ± 36 mg/h using a spark discharge under Ar, N2, and air, respectively. It was found that the energy dissipated in the spark gap is not a significant parameter that determines the mass production rate. Stable Pt nano-ink (25 wt.%) was prepared only on the basis of PtNPs synthesized under air. Narrow (about 30 μm) and conductive Pt lines were formed by the aerosol jet printing with prepared nano-ink. The resistivity of the Pt lines sintered at 750 °C was (1.2 ± 0.1)·10−7 Ω·m, which is about 1.1 times higher than that of bulk Pt. [ABSTRACT FROM AUTHOR]