Using the Vector LInearized Discrete Ordinate Radiative Transfer (VLIDORT) code as the main driver for forward model simulations, a first-of-its-kind data assimilation scheme has been developed for assimilating Ozone Monitoring Instrument (OMI) aerosol index (AI) measurements into the Naval Aerosol Analysis and Predictive System (NAAPS). This study suggests that both root mean square error (RMSE) and absolute errors can be significantly reduced in NAAPS analyses with the use of OMI AI data assimilation when compared to values from NAAPS natural runs. Improvements in model simulations demonstrate the utility of OMI AI data assimilation for aerosol model analysis over cloudy regions and bright surfaces. However, the OMI AI data assimilation alone does not outperform aerosol data assimilation that uses passive-based aerosol optical depth (AOD) products over cloud-free skies and dark surfaces. Further, as AI assimilation requires the deployment of a fully multiple-scatter-aware radiative transfer model in the forward simulations, computational burden is an issue. Nevertheless, the newly developed modeling system contains the necessary ingredients for assimilation of radiances in the ultraviolet (UV) spectrum, and our study shows the potential of direct radiance assimilation at both UV and visible spectrums, possibly coupled with AOD assimilation, for aerosol applications in the future. Additional data streams can be added, including data from the TROPOspheric Monitoring Instrument (TROPOMI), the Ozone Mapping and Profiler Suite (OMPS), and eventually the Plankton, Aerosol, Cloud and ocean Ecosystem (PACE) mission.