Synchronized sun-photometric measurements from the AERONET-CIMEL (AErosol RObotic NETwork) and GAW-PFR (Global Atmospheric Watch–Precision Filter Radiometer) aerosol networks are used to compare retrievals of the aerosol optical depth (AOD), effective radius, and volume concentration during a high-temporal-resolution measurement campaign at the Athens site in the Mediterranean Basin from 14 to 22 July 2009. During this period, direct-sun AOD retrievals from both instruments exhibited small differences in the range 0.01–0.02. The AODs measured with CIMEL and PFR instruments were inverted to retrieve particle microphysical properties using the linear estimation (LE) technique. For low aerosol loads (AOD < 0.2), measurements of the effective radius by the PFR were found to be −20% to +30% different from CIMEL values for both direct-sun data and inversion data. At higher loads (AOD > 0.4), measurements of the effective radius by the PFR are consistently 20 % lower than CIMEL for both direct-sun and inversion data. Volume concentrations at low aerosol loads from the PFR are up to 80% higher than the CIMEL for direct-sun data but are up to 20% lower when derived from inversion data under these same conditions. At higher loads, the percentage difference in volume concentrations from the PFR and CIMEL is systematically negative, with inversion data predicting differences 30% lower than those obtained from direct-sun data. An assessment of the effect of errors in the AOD retrieval on the estimation of PFR bulk parameters was performed and demonstrates that it is possible to estimate the particle volume concentration and effective radius with an uncertainty < 65% when AOD < 0.2 and when input errors are as high as 10%.