AbstractDaytime spectral sky radiance, or sky brightness, is deceptively complex to predict accurately. The Laser Environmental Effects Definition and Reference (LEEDR) first-principles atmospheric model propagates the spectral radiance of the sun to a sensor by modeling the scattering, absorption, and transmission of the radiated light through representative atmospheric layers. For this application, LEEDR was used to ingest numerical weather prediction (NWP) models, and scale the boundary layer and incorporate aerosol loading with ground-based measurements. This study compares LEEDR-derived spectral sky radiance simulations that include measured climatological, measured meteorological, and aerosol loading data to direct sky radiance measurements. Direct measurements of the daytime sky are accomplished with a 1-m-aperture telescope and simultaneous I-band and J-band camera observations (~0.8 and ~1.2 μm, respectively). LEEDR models of the daytime sky are compared to I-band and J-band radiances at multiple azimuths, elevations, and observation times. Residual error analysis is used to determine the accuracy of models including numerical weather prediction data, historical climatology, scaled aerosol loading via in situ particle count measurements, and meteorological updates. Key findings motivate the inclusion of real-time particle count measurements into future daytime sky radiance models for increased scattering accuracy via realistic atmospheric aerosol loading.