Mineral dust suspended in the atmosphere has significant effects on radiative balance and climate change. The Chinese Loess Plateau (CLP) is generally considered one of the main sources of Asian dust aerosol. After being lifted by wind, dust particles with various size distributions can be transported over different distances. In this study, an original loess sample was collected from Luochuan, which is centrally located on the CLP, and two samples with different size distributions were obtained afterwards. “Pristine loess” was used to represent dust that only affects source regions, part of pristine loess was milled to finer “milled loess” that can be transported over long distances. Light scattering matrices for these two samples were measured at 532 nm wavelength from 5 to 175^∘ angles. Particle size distribution, refractive index, chemical component, and microscopic appearance were also characterized for auxiliary analyses. Experimental results showed that there are obvious discrepancies in angular behaviors of matrix elements for pristine loess and milled loess, and these discrepancies are different from those for other kinds of dust with distinct size distributions. Given that the effective radii of these two loess samples differ by more than 20 times, it is reasonable to conclude that the difference in size distributions plays a major role in leading to different matrices, while differences in refractive index and microstructure have relatively small contributions. Qualitative analyses of numerical simulation results of irregular particles also validate this conclusion. Gaussian spheres may be promising morphological models for simulating the scattering matrix of loess but need further quantitative verification. Finally, synthetic scattering matrices for both pristine loess and milled loess were constructed over 0–180^∘, and the previous average scattering matrix for loess dust was updated. This study presents measurement results of Chinese loess dust and an updated average scattering matrix for loess, which are useful for validating existing models, developing more advanced models for optical simulations of loess dust, and helping to improve retrieval accuracy of dust aerosol properties over both source and downwind areas.