The mesoscale variability of dimethyl sulfide (DMS) and ocean color is explored to determine the feasibility of a predictive relationship. During NASA's Global Tropospheric Experiment/Chemical Instrumentation Test and Evaluation (GTE/CITE 3), simultaneous shipboard and aircraft studies were carried out in the North Atlantic, followed by aircraft studies in the South Atlantic. Surface concentrations of chlorophyll a were measured with an airborne spectroradiometer, the Ocean Data Acquisition System (ODAS), with simultaneous determinations of tropospheric DMS. Shipboard measurements of DMS in air and water as well as in situ chlorophyll a were taken in the North Atlantic. No relation was observed between shipboard aquatic DMS and chlorophyll a or primary productivity. Higher levels of aqueous DMS were not always reflected by atmospheric DMS, although shipboard and aircraft measurements of atmospheric DMS agreed very well. A significant relationship between atmospheric DMS and ocean color was seen once at low altitudes in both the North and South Atlantic only under clean air conditions. Atmospheric DMS levels during the North Atlantic experiment were probably lowered by the presence of mostly polluted air masses in the study area and were, overall, probably not representative of the in situ sea-to-air flux of DMS. Changes in concentration of aircraft-sensed chlorophyllous pigments were not reflected by atmospheric DMS. If a predictive algorithm is to be found, phytoplankton blooms should probably be the first place to study an ocean color-DMS relationship.