jats:titleAbstract</jats:title>jats:pDimethyl sulfide (DMS) is the largest source of natural sulfur in the atmosphere and undergoes oxidation reactions resulting in gas‐to‐particle conversion to form sulfate aerosol. Climate models typically use independent chemical schemes to simulate these processes, however, the sensitivity of sulfate aerosol to the schemes used by CMIP6 models has not been evaluated. Current climate models offer oversimplified DMS oxidation pathways, adding to the ambiguity surrounding the global sulfur burden. Here, we implemented seven DMS and sulfate chemistry schemes, six of which are from CMIP6 models, in an atmosphere‐only Earth system model. A large spread in aerosol optical depth (AOD) is simulated (0.077), almost twice the magnitude of the pre‐industrial to present‐day increase in AOD. Differences are largely driven by the inclusion of the nighttime DMS oxidation reaction with NOjats:sub3</jats:sub>, and in the number of aqueous phase sulfate reactions. Our analysis identifies the importance of DMS‐sulfate chemistry for simulating aerosols. We suggest that optimizing DMS/sulfur chemistry schemes is crucial for the accurate simulation of sulfate aerosols.</jats:p>