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Abstract This study considers the impact of electron precipitation from Earth's radiation belts on atmospheric composition using observations from the NASA Van Allen Probes and NSF Focused Investigations of Relativistic Electron Burst Intensity, Range, and Dynamics (FIREBIRD II) CubeSats. Ratios of electron flux between the Van Allen Probes (in near‐equatorial orbit in the radiation belts) and FIREBIRD II (in polar low Earth orbit) during spacecraft conjunctions (2015–2017) allow an estimate of precipitation into the atmosphere. Total Radiation Belt Electron Content, calculated from Van Allen Probes RBSP‐ECT MagEIS data, identifies a sustained 10‐day electron loss event in March 2013 that serves as an initial case study. Atmospheric ionization profiles, calculated by integrating monoenergetic ionization rates across the precipitating electron flux spectrum, provide input to the NCAR Whole Atmosphere Community Climate Model in order to quantify enhancements of atmospheric HO_xand NO_xand subsequent destruction of O₃in the middle atmosphere. Results suggest that current APEEP parameterizations of radiation belt electrons used in Coupled Model Intercomparison Project may underestimate the duration of events as well as higher energy electron contributions to atmospheric ionization and modeled NO_xconcentrations in the mesosphere and upper stratosphere.