Surface measurements of total and diffuse UV irradiance at the seven narrowband wavelength channels of the ultraviolet multifilter rotating shadow-band radiometer (UVMFR) were used to determine total column ozone and aerosol optical depth for two 6-month periods in 1997 and 1999 at a site in the Blue Ridge Mountains of North Carolina. The retrieved column ozone displayed a seasonal dependence and consistent agreement with the Total Ozone Mapping Spectrometer (TOMS). The mean ratio of retrieved ozone to TOMS ozone was 0.98 with standard deviations of 0.02 and 0.01 for 1997 and 1999, respectively. Aerosol optical depth at 317, 325, 332, and 368 nm was derived for a 6-month period of 1999. The seasonal trend exhibited is influenced by the persistent summertime haze that occurs in the region. The retrieved aerosol optical depths are used as input in a radiative transfer model to investigate the effect of their realistic values on the calculation of the UV index (UVI) forecasted by the National Weather Service. The percentage change in calculated surface erythemally weighted UV (versus calculations using the standard UVI aerosol inputs) ranges from a 4% increase to a nearly 50% decrease, dependent upon the aerosol optical depth and amount of absorption by aerosols. Based on our measurements, it was found that during the summertime the UV index can deviate by up to −5 index units from the forecast using the standard aerosol inputs.