AbstractMost ionospheric models cannot sufficiently reproduce the observed electron density profiles in the E‐region ionosphere, since they usually underestimate electron densities and do not match the profile shape. Mitigation of these issues is often addressed by increasing the solar soft X‐ray flux which is ineffective for resolving data‐model discrepancies. We show that low‐resolution cross sections and solar spectral irradiances fail to preserve structure within the data, which considerably impacts radiative processes in the E‐region, and are largely responsible for the discrepancies between observations and simulations. To resolve data‐model inconsistencies, we utilize new high‐resolution (0.001 nm) atomic oxygen (O) and molecular nitrogen (N2) cross sections and solar spectral irradiances, which contain autoionization and narrow rotational lines that allow solar photons to reach lower altitudes and increase the photoelectron flux. This work improves upon Meier et al. (2007, https://doi.org/10.1029/2006gl028484) by additionally incorporating high‐resolution N2 photoionization and photoabsorption cross sections in model calculations. Model results with the new inputs show increased O+ production rates of over 500%, larger than those of Meier et al. (2007, https://doi.org/10.1029/2006gl028484) and total ion production rates of over 125%, while production rates decrease by ∼15% in the E‐region in comparison to the results obtained using the cross section compilation from Conway (1988, https://apps.dtic.mil/sti/pdfs/ADA193866.pdf). Low‐resolution molecular oxygen (O2) cross sections from the Conway compilation are utilized for all input cases and indicate that is a dominant contributor to the total ion production rate in the E‐region. Specifically, the photoionization contributed from longer wavelengths is a main contributor at ∼120 km.