Optical models have been proposed to relate spectral variations in the beam attenuation (cp) and optical backscattering (bbp) coefficients to marine particle size distributions (PSDs). However, due to limited PSD data, particularly in the open ocean, optically derived PSDs suffer from large uncertainties and we have a poor empirical understanding of the drivers of spectral cp and bbp coefficients. Here we evaluated PSD optical proxies and investigated their drivers by analyzing an unprecedented dataset of co-located PSDs, phytoplankton abundances and optical measurements collected across the upper 500 m of the Atlantic Ocean. The spectral slope of cp was correlated (r>0.59) with the slope of the PSD only for particles with diameters >1 µm and also with eukaryotic phytoplankton concentrations. No significant relationships between PSDs and the spectral slope of bbp were observed. In the upper 200 m, the bbp spectral slope was correlated to the light absorption by particles (ap; r<-0.54) and to the ratio of cyanobacteria to eukaryotic phytoplankton. This latter correlation was likely the consequence of the strong relationship we observed between ap and the concentration of eukaryotic phytoplankton (r=0.83).