A multitude of sensitivity studies in the literature point to the importance of proper chemical and morphological characterization of particles when the radiative impacts of airborne dusts are modeled. However, the community data set is based on heterogeneous measurement methods relying on varying aerodynamic, chemical, morphological, and optical means. During the Puerto Rico Dust Experiment, size distributions of dust particles from Africa were measured using a variety of aerodynamic, optical, and geometric means. Consistent with the literature, comparisons of these size distributions showed quite dissimilar results. “Measured” volume median diameters varied from 2.5 to 9 μm for various geometric, aerodynamic, optical, and optical inversion methods. Aerodynamic systems showed mixed performance. Column integrated size distributions inverted from AERONET Sun/sky radiance data produced somewhat reasonable results in the coarse mode when given proper constraints and taken in the proper context. The largest systematic errors were found in optical particle counters due to insensitivities to particle size in the 4–10 μm region with further complications due to dust particle morphology and index of refraction issues. As these methods can produce quite dissimilar size distributions, considerable errors in calculated radiative properties can occur if incorrectly modeled into dust parameters. None of the methods compared in this study can adequately reproduce the measured mass extinction or mass scattering efficiency of the dust using spherical geometry methods. Given all of the uncertainties in the sizing methods, we promote the use of fundamental and quantifiable descriptors of particles such as mass as a function of aerodynamic diameter.