Nearly simultaneous measurements of the physical and optical properties of mixed layer and free tropospheric aerosols near Boulder, Colorado, were made on several occasions using aircraft, balloon, and ground‐based sensors. This effort (Front Range Lidar, Aircraft, and Balloon experiment (FRLAB)) was conducted with the purpose of obtaining a diverse, self‐consistent data set that could be used for testing optical model calculations based on measured physical characteristics such as apparent size distribution, composition, and shape. It was found that even with the uncertainties involved, the model predictions are in good agreement with the measurements in the visible and near infrared wavelength regions. At CO2 lidar wavelengths there is considerably more uncertainty in both the calculated and measured values; however, within the estimated errors there appears to be satisfactory agreement except for the highest free tropospheric layer studied. The results also indicate that during FRLAB the aerosol in the boundary layer and free troposphere behaved as spherical particles for optical modeling purposes. The utility of the observations for determining the extinction‐to‐backscatter ratio relevant to aerosols in the boundary layer and free troposphere is described with typical measured values being in the 20 to 30 sr range.