Aerosols play an important role in the Earth–atmosphere system. Their impacts on the weather and climate are highly dependent on spatiotemporal distributions as well as physical-optical properties. Physical-optical properties of the aerosols over the Asian continent have been widely investigated, but there are relatively few observations in maritime locations, especially the South China Sea (SCS). Here, with the combination of in situ ship-based observations from June and July 2019 as well as long-term MERRA-2 reanalysis datasets from January 2012 to December 2021, the physical and optical properties of marine aerosols in the SCS are explored. The impacts of meteorological factors, particularly frontal systems, on the aerosol properties are further analyzed based on detailed observations. The observed results show that aerosols are vertically concentrated below 3 km and the extinction coefficient reaches the maximum value of 0.055 km−1 near 480 m. Moreover, the particles are composed of an accumulation and a coarse particle mode, and they conform to the lognormal distribution. The synoptic-scale case study demonstrates that both the cold front and stationary front lead to an increase in aerosol optical thickness (AOD), which is due to the enhanced wind speed and the hygroscopic growth of fine particles, respectively. The long-term analysis indicates that AOD decreases from northwest to southeast with the increasing distance away from the continent, and it reflects higher values in spring and winter than in summer and autumn. Sulfate and sea salt dominate AOD in this region when compared with other components. The overall AOD shows a significant negative trend of −0.0027 year−1. This work will help us further understand the physical and optical properties of marine aerosols over the SCS and then contribute to quantifying the aerosol radiative forcing in the future.