Polarized light scattering measurements have the potential to provide improved characterization of natural particle assemblages in terms of particle size and composition. However, few studies have investigated this possibility for natural assemblages of marine particles. In this study, seawater samples representing contrasting assemblages of particles from coastal environments have been comprehensively characterized with measurements of angle-resolved polarized light scattering, particle size distribution, and particle composition. We observed robust trends linking samples containing higher proportions of large-sized particles with lower values of the maximum degree of linear polarization and the second element of the scattering matrix at a scattering angle of 100°, p22(100∘). In contrast, lower values of p22(20∘) were found in more non-phytoplankton-or inorganic--dominated samples. We also determined that three measurements involving the combinations of linearly polarized incident and scattered beams at two scattering angles (110° and 18°) have the potential to serve as useful proxies for estimating particle size and composition parameters.