© 2018 by the authors. The light scattering properties of seawater play important roles in radiative transfer in the ocean and optically-based methods for characterizing marine suspended particles from in situ and remote sensing measurements. The recently commercialized LISST-VSF instrument is capable of providing in situ or laboratory measurements of the volume scattering function, βp(Ψ), and the degree of linear polarization, DoLPp(Ψ), associated with particle scattering. These optical quantities of natural particle assemblages have not been measured routinely in past studies. To fully realize the potential of LISST-VSF measurements, we evaluated instrument performance, and developed calibration correction functions from laboratory measurements and Mie scattering calculations for standard polystyrene beads suspended in water. The correction functions were validated with independent measurements. The improved LISST-VSF protocol was applied to measurements of βp(Ψ) and DoLPp(Ψ) taken on 17 natural seawater samples from coastal and offshore marine environments characterized by contrasting assemblages of suspended particles. Both βp(Ψ) and DoLPp(Ψ) exhibited significant variations related to a broad range of composition and size distribution of particulate assemblages. For example, negative relational trends were observed between the particulate backscattering ratio derived from βp(Ψ) and increasing proportions of organic particles or phytoplankton in the particulate assemblage. Our results also suggest a potential trend between the maximum values of DoLPp(Ψ) and particle size metrics, such that a decrease in the maximum DoLPp(Ψ) tends to be associated with particulate assemblages exhibiting a higher proportion of large-sized particles. Such results have the potential to advance optically-based applications that rely on an understanding of relationships between light scattering and particle properties of natural particulate assemblages.