Dimethylsulfide (DMS) is biologically produced in the surface ocean and is the dominant natural source of sulfur to the atmosphere. Although DMS is an algal by-product, the ratio of DMS to chlorophyll (DMS:Chl) varies widely in the surface ocean. This is presumably because dimethylsulfoniopropionate (DMSP), the major precursor of DMS, DMSP-lyases, which catalyze the conversion of DMSP to DMS, and Chl vary as well with taxonomic composition than with the physiological state of the algal assemblage. Here we use remote sensing of Chl and phytoplankton dominance from PHYSAT with in-situ measured DMS concentrations to assess on an unprecedented spatial scale the affect of species composition on the DMS:Chl ratio in the surface ocean. Meridional distributions at 22° W in the Atlantic, and 95° W and 110° W in the Pacific, showed the same marked drop in DMS:Chl ratios near the equator, down to few mmol g−1, yet the basins exhibited different species dominance signatures. Hence, our results suggest that species composition was of secondary importance in controlling DMS and DMS:Chl variations in equatorial upwellings as well as physiological shifts in algal DMS production since mixed layer growth conditions (i.e., nutrient stress, temperature and light) were relatively homogeneous over the eastern equatorial Pacific. In the Indian sector of the Southern Ocean, warm core eddies with contrasting PHYSAT signatures displayed similar DMS levels. However, DMS:Chl ratios in eddies dominated by Synechococcus (SYN) were about 50% lower than that found in eddies showing nanoeucayotes or Phaeocystis-like signatures. DMS:Chl ratios varied with latitude in SYN dominated regions with ratios at low latitudes (away from equatorial upwellings) about twice that found at high northern and southern latitudes. This is the sole piece of coherent observations which indicates that species composition and growth conditions affect the large-scale dynamics of the DMS:Chl ratio. Overall, it appears that the DMS:Chl ratio is not consistent within specific phytoplankton groups determined from space. So DMS concentrations can not be derived from water-leaving radiance spectra obtained simultaneously from ocean color sensor measurements of Chl concentrations and dominant phytoplankton functional types. To proceed with the global investigation and better discriminate between factors affecting DMS:Chl ratios in the surface ocean, we recommend the use of PHYSAT records with higher spatial resolution in conjunction with other satellite products (e.g. particulate backscattering coefficients and indices of phytoplankton physiology and bloom status).