The Yellow Sea Large Marine Ecosystem (YSLME) is an important socioeconomic zone in Asia, but has been deteriorated by various environmental pollutants over the last half century. However, comprehensive coastal pollution assessments, particularly for heavy metals (HMs), have been limited from an international perspective. Here, we first evaluate coastal HM pollution in sediment and water from 119 riverine, estuarine, and marine locations along the BS and Yellow Sea to perform a comparative assessment between the two countries of China and South Korea. The occurrence, distribution, sources, multimedia fate, interactions, associated environmental factors, and potential ecological risks relating to the HM pollution are widely addressed. Eight typical HMs (As, Hg, Zn, Cu, Pb, Cd, Cr, and Ni) were targeted in both sediments and water, and in situ water properties (pH, dissolved oxygen, salinity, and temperature) and sediment properties (pH and organic matter (OM) content) were analyzed. The results indicated that As, Cd, Cr, Cu, Ni, and Pb concentrations in water were higher in the estuarine area than those in riverine and marine areas and that particularly severe HM pollution was evidenced in the BS. The dominant elements in pollution hot spots varied greatly among the countries and regions. According to the geo-accumulation index (Igeo) and pollution load index (PLI) values, the sediments exhibited high Hg and Pb pollution in the BS; high As, Hg, and Pb pollution in the Yellow Sea of China; and high Cd and Hg pollution in the Yellow Sea of South Korea. In general, the sediments were moderately contaminated by HMs based on the high PLI (>1.0) and risk index (RI) values (>160). Ni and Cr in the sediment mainly originated from geogenic sources, while the other elements (Zn, As, Cd, Cu, Hg, and Pb) were primarily linked to anthropogenic sources. Based on the partial redundancy analysis, we found that environmental factors, especially OM, contributed significantly to the concentrations of HMs in both the sediments and water. The sediment HMs significantly contributed to the waterborne HMs due to their release from the sediments to the water column. An overall assessment of the contamination status, spatial distribution, and potential sources of HMs suggested that the water-sediment interaction of HMs and the influence by environmental factors should be subsequently considered for a better understanding of the multimedia fate of HMs in the given dynamic YSLME system or similar environments elsewhere.