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In this study, spatiotemporal heterogeneities in the concentrations of alkaline gases and their particulate counterparts in the marine atmosphere over China's marginal seas were investigated in terms of causes and chemical conversion during two winter cruise campaigns, using semi-continuous measurements made by an onboard URG-9000D Ambient Ion Monitor-Ion chromatograph (AIM-IC, Thermofisher). During the cruise campaign over the East China Sea on December 27, 2019–January 6, 2020, the concentrations of atmospheric trimethylamine (TMAgas) varied by approximately one order of magnitude, with an average (±standard deviation) of 0.10 ± 0.04 µg m−3. Corresponding means were 0.037 ± 0.011 µg m−3 over the Yellow Sea on 7–16 January 2020 and 0.031 ± 0.009 μg m−3 over the Yellow Sea and the Bohai Sea on 9–22 December 2019. In contrast, the simultaneously observed concentrations of TMA in PM2.5, detected as TMAH+, over the East China Sea were 0.098 ± 0.068 µg m−3 and substantially smaller than 0.28 ± 0.18 μg m−3 over the Yellow Sea and the Bohai Sea on 9–22 December 2019. A significant correlation between TMAgas and particulate TMAH+ was obtained over the East China Sea, but no correlation existed over the Yellow Sea and Bohai Sea. The proportional or disproportional variations in concentrations of TMAgas with particulate TMAH+ over the sea zones were likely attributed to the difference in enrichment of TMAH+ in the sea surface microlayer. In addition, spatiotemporal heterogeneities in concentrations of atmospheric ammonia (NH3gas), atmospheric dimethylamine (DMAgas), and DMA in PM2.5, detected as DMAH+, were also investigated. Case analyses were performed to illustrate the formation and chemical conversion of particulate aminium ions in marine aerosols. Finally, we hypothesized a release of basic gases and particulate counterparts from the ocean to the atmosphere, together with secondary formation of DMAH+ and chemical conversion of TMAH+, in the marine atmosphere.