Sulfur development in water-sediment systems is closely related to eutrophication and harmful algae blooms (HABs). However, the development of sulfur in water-sediment systems during heavy algae accumulation still remains unclear, especially in hyper-eutrophic shallow lakes. In this study, a quarterly field investigation was carried out for a year in the algae accumulated embay area of Lake Taihu, accompanied by a short-term laboratory experiment on algae accumulation. The results show that hydrogen sulfide and methanethiol dominated the volatile sulfur compounds (VSCs) in the water during non-accumulation seasons, whereas the concentrations of dimethyl sulfides increased during heavy algae accumulation, both in the field and the laboratory. An increase in the acid volatile sulfide (AVS) in the surface sediments was also discovered together with the increase in dimethyl sulfides. The depletion of oxygen in the overlying water and sediment-water interface during the heavy algae accumulation and decomposition was found to be closely related to both the increase in VSCs in the overlying water and increase in AVS in the sediment. The increased concentrations of these reductive sulfocompounds might aggravate the eutrophication and HABs and should be given more consideration in future eutrophication control plans for lakes.2 of 15 of P to phytoplankton increases when the release of P from the sediments increases under anoxic conditions [20,21]; this usually occurs during algal blooms [22][23][24]. The formation of sulfides facilitates the formation of ferrous sulfide (FeS) and the release of P from the sediments [14], aggravating eutrophication and HABs in the water. This process usually takes place in freshwater sediments because of the low sulfate concentration of freshwater [14,25]. However, in the overlying water, another problem is the formation of volatile sulfur compounds (VSCs) during HABs. Various VSCs, including hydrogen sulfide (H 2 S), methanethiol (MTL), dimethyl sulfide (DMS), dimethyl disulfide (DMDS), and dimethyl trisulfide (DMTS), have been detected during HABs [26][27][28]. MTL, DMS, DMDS, and DMTS are also known as volatile organic sulfur compounds (VOSCs). The high concentration of VSCs causes freshwater sites to become more odorous [29,30]. In 2007, a crisis occurred in Wuxi City, China, resulting from the accumulation of algae in Lake Taihu, the city's drinking water source, in which the tap water turned black and became odorous [31,32]. High levels of VSCs were found to be responsible for the crisis [31,32]. VSCs are difficult to remove from drinking water sources through conventional techniques due to the high cost and the residual of the processes required [33]. Therefore, it is imperative to understand the origin and formation of VSCs in drinking water sources such as lakes and reservoirs.Although the formation and migration of sulfides and VSCs have been noted and studied worldwide [28,34], the development of these compounds in the water and sediment systems still remains unclear, especially...