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The impact of inorganic salts and organic matter (OM) on the production of primary marine aerosols is still under debate. To constrain their impact, we investigated primary aerosols generated by a sea-spray generator chamber using surface water samples from rivers, estuaries, and seas that were collected along salinity gradients in two temperate Korean coastal systems and one Arctic coastal system. Salinity values showed an increasing trend along the river–estuary–coastal water transition, indicating the lowest amount of inorganic salts in the river but the highest amount in the sea. In river samples, the lowest number concentration of primary aerosol particles (1.01 × 103 cm−3) was observed at the highest OM content, suggesting that low salinity controls aerosol production. Moreover, the number concentration of primary aerosols increased drastically in estuarine (1.13 × 104 cm−3) and seawater (1.35 × 104 cm−3) samples as the OM content decreased. Our results indicate that inorganic salts associated with increasing salinity play a much larger role than OM in aerosol production in river-dominated coastal systems. Laboratory studies using NaCl solution supported the conclusion that inorganic salt is a critical factor in modulating the particles produced from river water and seawater. Accordingly, this study highlights that inorganic salts are a critical factor in modulating the production of primary marine aerosols.