English: Sulfur, as an essential nutrient for plant growth, has increasingly been used in fertiliser applications for many crops. This increase is coincident with declines in atmospheric sulfur deposition in response to air quality improvements in the United States and Europe. Here, we evaluate trends in sulfur fertiliser sales by mass, as a proxy for fertiliser applications, and estimate total atmospheric sulfur deposition across the Midwestern United States. Crop acreage, yield and sulfur fertiliser application substantially increased between 1985 and 2015, coincident with declines in atmospheric sulfur deposition. The increase in sulfur fertiliser has outpaced the relative rate of change in other major nutrient fertilisers including nitrogen, phosphorus and potassium, by approximately 7-fold prior to 2009, and 29-fold after 2009. We suggest that there is a critical need to develop sulfur management tools that optimize fertiliser applications to maintain crop yields while minimizing the consequences of excess sulfur in the environment.