The proposed strong positive relationship between dimethylsulphide (DMS) concentration and the solar radiation dose (SRD) received into the surface ocean is tested using data from the Atlantic Meridional Transect (AMT) programme. In situ, daily data sampled concurrently with DMS concentrations is used for the component variables of the SRD (mixed layer depth, MLD, surface insolation, I0, and a light attenuation coefficient, k) to calculate SRDinsitu. This is the first time in situ data for all of the components, including k, has been used to test the SRD-DMS relationship over large spatial scales. We find a significant correlation (ρ=0.55 n=65 p<0.01) but the slope of this relationship (0.006 nM/W m−2) is less than previously found at the global (0.019 nM/W m−2) and regional scales (Blanes Bay, Mediterranean, 0.028 nM/W m−2; Sargasso Sea 0.017 nM/W m−2). The correlation is improved (ρ=0.74 n=65 p<0.01) by replacing the in situ data with an estimated I0 (which assumes a constant 50% removal of the top of atmosphere value; 0.5×TOA), a MLD climatology and a fixed value for k following previous work. Equally strong, but non-linear relationships are also found between DMS and both in situ MLD (ρ=0.61 n=65 p<0.01) and the estimated I0 (ρ=0.73 n=65 p<0.01) alone. Using a satellite-retrieved, cloud-adjusted surface UVA irradiance to calculate a UV radiation dose (UVRD) with a climatological MLD also provides an equivalent correlation (ρ=0.67 n=54 p<0.01) to DMS. With this data, MLD appears the dominant control upon DMS concentrations and remains a useful shorthand to prediction without fully resolving the biological processes involved. However, the implied relationship between the incident solar/ultraviolet radiation (modulated by MLD), and sea surface DMS concentrations, is critical for closing a climate feedback loop.