Nowadays, plant invasion has become a global ecological threat to local biodiversity and ecosystem stability. Spartina alterniflora encroaches on the ecological niches of local species and changes the soil’s nutrient cycle. However, few comprehensive assessments focus on the effects of S. alterniflora invasion. Here, we investigated how soil sulfur changed with spatiotemporal variation and life forms of native species after S. alterniflora invasion and speculated the possible mechanism of the sulfur increase based on the references. The invasion of S. alterniflora increased soil total sulfur by 57.29% and phytotoxic sulfide by 193.29%. In general, the invasion of S. alterniflora enhanced the total plant biomass and soil nutrients, e.g., soil organic carbon, total nitrogen, and soil microbial biomass carbon, further increasing soil sulfur content. The sulfur accumulation caused by S. alterniflora might result in the poisoning of native species. Thus, we hypothesized that the success of S. alterniflora invasion was closely connected with soil sulfur, especially toxic sulfide. Our study suggests that researchers should give more attention to the correlation between S. alterniflora invasion and the soil sulfur increase. More research is needed to investigate the mechanisms of the successful invasion by accumulating phytotoxic sulfide.